Adv Funct Materials - 2022 - Ling - Emerging MXene Based Memristors For in Memory Neuromorphic Computing and Logic

Review
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Emerging MXene-Based Memristors for In-Memory,

Neuromorphic Computing, and Logic Operation
Songtao Ling, Cheng Zhang,* Chunlan Ma, Yang Li,* and Qichun Zhang*
and predicted to reach ≈100 ZB by 2023.[1]

Confronted by the difficulties of the von Neumann bottleneck and memory The rapid development of modern infor-
wall, traditional computing systems are gradually inadequate for satisfying mation industry has put forward higher
the demands of future data-intensive computing applications. Recently, demands for memory and data storage
memristors have emerged as promising candidates for advanced in-memory technology, such as minimization, fast
speed, low power consumption, and high
and neuromorphic computing, which pave one way for breaking through the
storage capacity.[2,3] However, the tradi-
dilemma of current computing architecture. Till now, varieties of functional tional computing systems adopt von Neu-
materials have been developed for constructing high-performance memris- mann architecture, where the memory
tors. Herein, the review focuses on the emerging 2D MXene materials-based and central processing unit are sepa-
memristors. First, the mainstream synthetic strategies and characterization rately located with linear interactions.[4,5]
This complex systemic configuration
methods of MXenes are introduced. Second, the different types of MXene-
often results in slow data transfer and
based memristive materials and their widely adopted switching mechanisms high power consumption, which con-
are overviewed. Third, the recent progress of MXene-based memristors for fronts inevitable difficulties of von Neu-
data storage, artificial synapses, neuromorphic computing, and logic circuits mann bottleneck and memory wall.[6–11]
is comprehensively summarized. Finally, the challenges, development trends, To address these issues, the development
and perspectives are discussed, aiming to provide guidelines for the prepa- of new-generation data storage and com-
puting technology becomes more urgent
ration of novel MXene-based memristors and more engaging information
than ever.[12,13]
technology applications. Recently, memristors, which were theo-
retically proposed by Leon Chua[14] and
first demonstrated by Hewlett Packard lab-
1. Introduction oratory,[15] have aroused tremendous attention due to the advan-
tages of excellent data storage capability, low operating energy,
With the advent of Big Data era and Internet of Things, the fast response, and in-memory computing potential.[16–20] Dif-
amount of global digital information has been ever-increasing ferent from the traditional Flash memory and random-access
memory that rely on charges, memristors can alter their resist-
ances to the history of electrical input, offering the media to
S. Ling, C. Zhang, C. Ma, Y. Li
Jiangsu Key Laboratory of Micro and Nano Heat Fluid Flow Technology
store information in the form of resistance switching.[21–23]
and Energy Application Moreover, memristors with reconfigurable history-dependent
School of Physical Science and Technology resistive switching behaviors show great promise to mimic
Suzhou University of Science and Technology biological synapses, which emerge as one of the most fasci-
Suzhou, Jiangsu 215009, China nating technologies for implementing artificial neural network
E-mail: zhangcheng@usts.edu.cn; liyang@usts.edu.cn
for neuromorphic computing.[24–28] Attributing to these glaring
Y. Li
The Key Laboratory of Synthetic and Biological Colloids merits, varieties of materials have been widely explored for
Ministry of Education memristors construction and application. Among these, 2D
Jiangnan University materials have aroused particular interests because of their
Wuxi, Jiangsu 214122, China unique structures and optoelectronic properties.[29–32]
Q. Zhang 2D materials are the material family that integrate by strong
Department of Materials Science and Engineering
City University of Hong Kong
in-plane chemical bonds and relatively weak out-of-plane van der
Kowloon, Hong Kong SAR 999077, China Waals interactions.[33–38] The atomic thickness of 2D materials
E-mail: qiczhang@cityu.edu.hk offers an enormous advantage for realizing high-density inte-
Q. Zhang gration and fast-response processing of memristor devices.[39–41]
Center of Super-Diamond and Advanced Films (COSDAF) Moreover, their planar structures endow outstanding compat-
City University of Hong Kong ibility with conventional wafer semiconductor technology.[42,43]
Kowloon, Hong Kong SAR 999077, China
To date, 2D material-based memristors have witnessed great
The ORCID identification number(s) for the author(s) of this article
can be found under https://doi.org/10.1002/adfm.202208320.
progress in past decades.[30,44–46] In particular, it is noteworthy
that an emerging metal-based 2D material, namely MXene, has
DOI: 10.1002/adfm.202208320 exhibited an intriguing prospect for achieving high-performance
Adv. Funct. Mater. 2023, 33, 2208320 2208320 (1 of 23) © 2022 Wiley-VCH GmbH
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memristors.[47,48] MXenes are nanosheets of transition metal from the MAX phase using HF as etching agent, and obtained
carbides, nitrides, or carbonitrides, which are mainly produced Ti3C2Tx by extracting the weakly bound Al layer from precursor
by selectively etching A layers from Mn+1AXn (n = 1, 2, 3, and 4) Ti3AlC2 phase (Tx = OH and F). Since their first appear-
composites, where M is one or two of the early transition metal ances, MXenes have attracted extensive attention due to the
elements, A is a group IIIA or IVA element, and X is C and/ appealing physical and chemical properties such as metal-like
or N.[49–51] During the etching process of A layer from Mn+1AXn conductivity, hydrophilicity, and tunable functional groups at
phase, the broken MA bond can spontaneously interact with the surface. The family of MXenes has grown rapidly in the past
anions in different etching solutions and form surface termi- decade. Meanwhile, various synthetic strategies for MXenes
nated groups of Tx (e.g., OH, F, Cl, O).[52–54] Therefore, have been proposed, including “top-down” and “bottom-up”
the general chemical formula of MXenes is Mn+1XnTx. Compared methods (Figure 2a). Among them, the “top-down” strategy is
with other materials like metal oxides, the abundant Tx groups to exfoliate bulk materials (e.g., MAX phase) into several layers,
of OH and O endow MXenes with satisfactory hydrophility, which are usually obtained by selective etching of element A
which can facilitate the manufacturing process through simple, with appropriate etching agents. The etching methods contain
versatile, and low-cost solution-processed techniques. Moreover, acid (e.g., HF,[83,84] H3PO4,[85]) NH4HF2,[86,87] molten salt (e.g.,
their 2D nanosheet structure and solution-processable prop- LiF+KF,[88] ZnCl2,[89]) Alkali (NaOH,[90]) and fluoride salt+HCl
erty are favorable for fabricating high-performance flexible (e.g., LiF,[91] KF,[92] NH4F.[90]) The “bottom-up” strategy is to uti-
electronics. Recently, more than twenty kinds of MXenes with lize chemical vapor deposition (CVD) technique to grow MXene
Mn+1XnTx form have been experimentally synthesized, for which films on the substrate surface. Due to the different synthetic
the elementary compositions are illustrated in the periodic table strategies, the physical and chemical properties of MXenes are
(Figure 1a). Thanks to their excellent chemical, mechanical, and usually distinct. Meanwhile, the properties of 2D MXenes also
electrical properties, 2D MXene materials have exhibited broad largely depend on their starting materials and various surface
prospects in the fields of supercapacitors,[55,56] electromag- modification methods. Therefore, it is necessary to under-
netic interference shielding,[57–60] sensors,[61,62] water purifica- stand the main synthetic steps of MXenes and figure out the
tion,[63–65] and electrocatalysis.[66–69] advantages and disadvantages of different strategies, which can
In this review, we focus on the recent advances of MXene- provide guidance for preparing MXenes with unique proper-
based materials for memristors, and their promising applica- ties for the memristor applications, including data storage,
tions for novel memory and computing technology.[18,70–72] artificial synapses, neuromorphic computing, and logic
Attributed to the great progress, it is vital to provide a timely circuits.
and comprehensive overview to systematically introduce the
latest research advances and versatile applications of MXene-
based memristors as well as their development trends. Never- 2.1. Top-Down
theless, a survey of studies reveals that such kinds of system-
atic reviews are relatively scarce,[47,48,73] which require more Figure 2b shows the structural diagram of Mn+1XnTx (n = 1–4),
research attention. Here, we are apt to offer a comprehensive where X atomic layers are alternately arranged between two
summary about the MXene-based memristive materials and tightly-packed M layers and X atoms occupy the octahedral
devices from preparation to application. The intention of this positions. Tx groups (e.g., OH, F, Cl, O) occupy the
review is to hasten more encouraging research achievements outer shell of the molecular structure, which are conducive
of MXene-based memristors for novel information technolo- to realizing the surface modification of MXenes. MXenes are
gies, and promote their practical applications in the upcoming synthesized by selective etching of element A in the MAX
artificial intelligent era. This review begins with an introduc- phase. As shown in Figure 2c, more than 20 kinds of MXenes
tion on the synthetic strategies and charaterization methods of with Mn+1XnTx (n = 1–4) structures have been reported to
MXenes, followed by the classifications of memristive mate- date. Currently, the established MXene series include M2X
rials and operational mechanisms of memristor devices. Then, (Ti2CTx,[93] Ti2NTx,[89,94] V2CTx,[95–97] V2NTx,[91] Nb2CTx,[98–100]
the diverse application scenarios of MXene-based memristors Ta2CTx,[101] Mo2CTx,[102,103] Cr2CTx[104,105]), M3X2 (Cr2TiC2Tx,[106]
are summarized, including data storage, artificial synapses, Mo2ScC2Tx,[106,107] Mo2TiC2Tx,[106,108] Ti3CNTx,[109,110] Hf3C2Tx,[111]
neuromorphic computing, and logic circuits, as illustrated in Ti3C2Tx,[94,112,113] Zr3C2Tx[114]), M4X3 (Mo2Ti2C3Tx,[108] Ta4C3Tx,[115]
Figure 1b. Finally, the challenges faced by MXene-based mem- V4C3Tx,[116,117] Nb4C3Tx,[118] Ti4N3Tx[88]), and M5X4 (Mo4VC4Tx[119]).
ristors, their potential solutions, development trends, and cor- More MXene materials are expected to be exfoliated from the
responding perspectives are outlined. Our review is aimed to MAX phases in the future. Notably, during the etching reaction
boost more research endeavors for achieving high-performance process, the outer surface of MXenes usually terminates with
MXene-based memristors, and provide methodical guidance OH, F, Cl, or O groups, which can be ascribed to the
for the further development of in-memory and neuromorphic spontaneous formation between the broken M-A weak metal
computing systems based on novel 2D materials. bond and anions in the etching solutions (represented as Tx,
where x represents the number of terminations).
For “top-down” synthetic technique, MXenes can be obtained
2. Synthetic Strategies of MXenes by etching MAX and non-MAX phases.[120–122] Different reac-
tion reagents and conditions may introduce different sur-
In 2011, Gogotis et al. from Drexel University first reported face groups and affect the morphology, stability, and electrical
the preparation of MXenes.[82] They selectively etched A layer properties of MXenes.[123,124] As illustrated in Figure 3a, Shuck
Figure 1. a) Elementary compositions of MXenes and MAX phases based on experimental research. M represents the early transition metal elements
(in light yellow). A is usually an IIIA or IVA element (in dark yellow). X is C and/or N (in blue), and T is surface terminal functional elements (in green).
b) The synthesis strategies of MXenes. Top-down. Reproduced with permission.[74] Copyright 2020, Wiley-VCH. Bottom-up. Reproduced with permis-
sion.[75] Copyright 2019, Wiley-VCH. The switching mechanisms of MXene-based memristors. Filamentary conduction. Reproduced with permission.[76]
Copyright 2021, American Chemical Society. Charge trapping. Reproduced with permission.[77] Copyright 2019, Royal Society of Chemistry. The appli-
cations of MXene-based memristors. Date storage. Reproduced with permission.[78] Copyright 2020, American Chemical Society. Artificial synapses.
Reproduced with permission.[79] Copyright 2019, Wiley-VCH. Neuromorphic computing. Reproduced with permission.[80] Copyright 2022, Elsevier. Logic
circuit. Reproduced with permission.[81] Copyright 2021, American Chemical Society.
et al. etched Ti3AlC2 with HF and HCl mixture. The reaction to provide a safer synthetic method, Ghidiu et al. reported a
solution was precipitated and repeatedly washed to make the method of preparing such material via fluoride salts (lithium
upper liquid neutral, and finally MXene of Ti3C2Tx was obtained fluoride) and HCl solution, which avoids the danger of han-
through vacuum filtration of Celgard membrane.[74] Although dling concentrated HF.[94] After etching, a clay-like precipitation
HF etching has been widely used in the preparation of Ti3C2Tx, is obtained, which can be dried into a thin film or other shaped
it requires additional HF post-processing procedures. In order electrodes.
Figure 2. a) Synthetic strategies for MXenes and the representative reagents used for selective etching of MAX phases or other precursor materials.
b) Schematic of Mn+1XnTx structures with n = 1–4. c) Schematic of experimentally synthesized MXenes.
2.2. Bottom-Up a “bottom-up” method.[125–127] Due to the absence of oxygen-

containing functional groups at their surfaces, the structures of
Due to the complex atomic compositions and structures of transition metal carbides/nitrides (such as Mo2C) produced by
MXene layers, the MXene sheets obtained by etching the MAX CVD are different from those of MXenes synthesized by “top-
phase with chemical regents (e.g., HF or fluoride salt + HCl) down” method. Such difference is similar to that between gra-
usually have small sizes (transverse sizes ranging from hun- phene and defective reduced graphene oxide.[128,129] Figure 3b,c
dreds of nanometers to 10 µm) and numerous structural represents the growth of large-area and high-quality 2D
defects. Chemical vapore deposition (CVD) is the typical ultrathin α-Mo2C crystals by CVD.[75] The obtained 2D ultrathin
“bottom-up” synthetic method to develop layered materials α-Mo2C materials possess different shapes, few structural
with high production quality. Compared with traditional defects, and anisotropy of strong magnetic field. This method
chemical etching, the MXene sheets with ultra-thin feature, adopts methane as carbon source and Cu/Mo foil as substrate.
large transverse size, and high quality can be synthesized by The 2D ultrathin α-Mo2C crystals deposited at 1100 °C can grow
Figure 3. a) Schematic of Ti3C2Tx synthesis. Reproduced with permission.[74] Copyright 2020, Wiley-VCH. Large-area 2D ultrathin α-Mo2C crystals fabri-
cated by CVD with different shapes of b) hexagonal shape, and c) “wedding cake” shape. Reproduced with permission.[75] Copyright 2019, Wiley-VCH.
into a large size with a transverse dimension over 100 µm and Raman peaks of Ti3C2Tx at 144, 263, 394, and 589 cm−1. The
a thickness of several nanometers. Overall, MXenes can be syn- XRD pattern was in accord with that of crystalline Ti3C2Tx
thesized by a variety of methods. Different methods can result flakes (Figure 4b), suggesting the good quality of as-prepared
in different structures and surface terminations, which affect Ti3C2Tx. The SEM image in Figure 4c presented the surface
the mechanical and electrical properties. Therefore, MXenes topography of Ti3C2Tx flakes in spin-coated film state. The XPS
can be selectively prepared using chemical etching or CVD curves verified the chemical compositions of Ti3C2Tx flakes
technique, in order to meet the requirements of the particular (Figure 4d–f). Sun et al. synthesized thin Ti3C2Tx nanosheets
applications such as memristors. and characterized their structures.[78] The TEM and SAED pat-
terns revealed that the Ti3C2Tx nanosheets possessed high crys-
tallinity and a well-crystallized hexagonal structure (Figure 4g).
3. Characterization of MXenes The AFM height profile showed that the thickness of Ti3C2Tx
nanosheet was ≈1.5 nm (Figure 4h). They further modified
The thorough characterization of the chemical composition Ti3C2Tx by octylphosphonic acid through surface chemistry
and microscopic structure of MXenes is very important for engineering. The high-resolution TEM (HRTEM) mapping
confirming their specific structures and understanding their indicated that phosphorus was uniformly distributed on the
intrinsic properties.[130,131] Recently, various methods have Ti3C2Tx nanosheets, which demonstrated that the surface
been adopted to characterize MXenes, including Raman spec- modification of MXene by octylphosphonic acid was feasible
troscopy, X-ray photoelectron spectroscopy (XPS), scanning (Figure 4i).
electron microscopy (SEM), atomic force microscopy (AFM),
powder X-ray diffraction (PXRD), transmission electron micro
scopy (TEM), and selected area electron diffraction (SAED). 4. MXene-Based Memristive Materials
Raman spectroscopy and XPS are the typical techniques for
investigating the chemical compositions of MXenes. SEM can Recently, a variety of MXene-based functional materials have
help to offer the microscopic visualization of MXene structures. been demonstrated for memristor applications, including
AFM is a widely-adopted characterization method for the anal- single-component Mn+1Xn, laminated heterostructures of
ysis of 2D MXene materials since it can provide information MXenes with other materials, and composite structures by
about both the lateral nanosheet dimensions and longitudinal chemical modification or physical adsorption (representa-
thickness. PXRD is a powerful technique to identify the forma- tive examples as listed in Table 1). Single-component Mn+1Xn
tion of MXenes, because when transforming the MAX phase to as memristive materials include V2C,[132–134] Ti3C2Tx,[76,135]
multilayer MXene, and then to delaminated MXene, the char- etc. Due to the different terminal Tx of MXenes and different
acteristics of PXRD patterns can change accordingly. TEM and adopted electrodes, the single-component MXene-based mem-
SAED are vital techniques to figure out the crystalline nature ristors can show diverse performances and applications. For
of MXene materials. By atomic resolution imaging method, example, Sokolov et al. fabricated a two-terminal memristor
the specific structure, arrangement, atomic distribution, and of Ag/Ti3C2Tx/Pt structure with the single-component Ti3C2Tx
related information can be obtained, affording both qualitative nanosheets as an active layer, which exhibited threshold resis-
and quantitative cognition of the MXene structures. These tech- tive switching characteristics and realized the versatile synaptic
niques cooperatively offer the structural information, which emulations including paired-pulse facilitation, post-tetanic
help to get insight into the microscopic properties of MXenes. potentiation, short-term potentiation, and short-term poten-
For example, Yan et al. prepared Ti3C2Tx MXene flakes for tiation to long-term potentiation transition.[135] For laminated
memristor application.[79] They characterized the Ti3C2Tx flakes MXene-based memristors, a strategy of preparing binary layered
through Raman spectroscopy, XRD, SEM, and XPS techniques. structures is to first deposit an oxygen-containing functional
As shown in Figure 4a, the dashed lines manifested the typical layer (e.g., SiO2[136,137] and TiO2[138]) onto the bottom substrate
Figure 4. a) Raman spectrum of Ti3C2Tx. b) XRD pattern of Ti3C2Tx. c) SEM image of the Ti3C2Tx film. XPS spectra of Ti3C2Tx: d) Ti 2p, e) C 1s, and
f) O 1 s. Reproduced with permission.[79] Copyright 2020, American Chemical Society. g) AFM image of Ti3C2Tx. h) TEM image of Ti3C2Tx (inset: SAED
pattern). i) HRTEM mapping of octylphosphonic acid-modified Ti3C2Tx monolayer. Reproduced with permission.[78] Copyright 2019, Wiley-VCH.
by physical vapor deposition (PVD), and then fabricate a layer the Ti3C2Tx-ZnO composite as active material, a multi-modal
of MXenes on the oxygen-containing functional layer. Another flexible sensing memristor was achieved, which was promising
strategy is proposed by Yang et al., which obtains a layer of for in-sensor computing application.
MoOx at the surface of Mo2C by thermal oxidation and affords
a vertical MoOx/Mo2C heterostructure.[139] MXene composites-
based materials have also been reported for memristive active 5. Memristive Switching Mechanisms
elements, including Ti3C2Tx-octylphosphonic acid (Ti3C2Tx-
OP), Ti3C2Tx-ZnO, Ti3C2-TiO2, etc. After modifying MXenes by Along with the development of high-performance MXene-
octylphosphonic acid[78] or nitrate (AgNO3, Zn(NO3)2∙6H2O) based memristive materials, the exploration of their underlying
solution,[80,140] the obtained MXene composites can achieve switching mechanisms is also very important for understanding
intriguing memristive properties. For instance, the Ti3C2Tx- the device performance. On the basis of theoretical calculation
ZnO composite was successfully prepared by slowly adding and experimental analysis, several mechanisms have been pro-
Zn(NO3)2∙6H2O aqueous solution into Ti3C2Tx nanosheets posed to explain the different memristive characteristics. Here,
suspension under vigorous stirring.[140] The hydrophilicity of we focus on the most common and widely accepted switching
2D Ti3C2Tx nanosheets facilitated the self-assembly of ZnO mechanisms in the field of MXene-based memristors, i.e., fila-
nanoparticles through the hydro-thermal method. By utilizing mentary conduction and charge trapping.
Table 1. Different kinds of MXene-based memristive materials and their applications.
Functional layer Structure Application Reference

One-component Ag/V2C/W data storage/neuromorphic computing [132–134]
Ag/Ti3C2Tx/Pt artificial synapse [76,135]
Cu/Ti3C2/Cu neuromorphic computing [141]
Al/Ti3C2Tx/Pt artificial synapse [76,79]
Pt/Ti3C2Tx/Pt data storage [76]
Laminated construction Ag/V2C/TiO2/W artificial synapse [138]
Pd/MoOX/Mo2C/Au data storage [139]
Ag/Ti3C2/SiO2/Pt artificial synapse [142]
Cu/Ti3C2/SiO2/W data storage/artificial synapse [136,137,143]
TiN/Cu/Ti3C2/SiO2/TiN artificial synapse/neuromorphic computing [144,145]
Composites Al/Ti3C2Tx-OP/ITO multilevel data storage [78]
ITO/Ti3C2-ZnO/Al in-sensor computing [140]
Au/Ti3C2Tx@PVP/rGO data storage [146]
Al/Ti3C2Tx@PVPy/ITO multilevel data storage [77]
Au/Ti3C2TxQDs@PVP/ITO data storage [147]
Al/Ti3C2@Ag/Pt neuromorphic computing [80]
Au/(AgNPs)Ti3C2-TiO2/ITO data storage/logic circuit [81]
5.1. Filamentary Conduction 5.1.2. Valence Change Memory (VCM)
The filamentary conduction is closely related to the active VCM forms conductive filaments through the movement of
materials and electrodes used in the memristor devices, which donor-type defects such as atomic vacancies in the active layer.
is generally considered to comprise two types of conduction Taking oxygen vacancy as an example, by applying external
modes. voltage, oxygen ions in the active layer will migrate to the
anode under the electrical driving force, leaving a large number
of oxygen vacancies. Thus, the oxygen vacancies gather at
5.1.1. Electrochemical Metallization Memory (ECM) the cathode and diffuse upward into the active layer, forming
anoxic filament and changing the conductivity of the device.
For two-terminal memristors, the active metals are usually Similar to ECM, VCM can exhibit reversible bipolar filament
adopted as the electrodes, such as Ag and Cu. By applying posi- switching behavior under opposite electric field. For example,
tive voltage bias to the top electrode, active electrode materials Khot et al. also fabricated a Pt/Ti3C2/Pt memristor in the
will lose electrons at the anode and become metal cations, same work, where inert metal Pt was used as the top electrode
which can be released from the top active electrode and trans- (Figure 5c).[76] The memristive mechanism of Pt/Ti3C2/Pt is
mitted downward through the active layer under the action of attributed to the back and forth movement of oxygen vacancies
electric field. These metal cations eventually reduce to metal in the active layer, leading to the formation and fracture of con-
atoms at the cathode and gradually accumulate upward to form ductive filaments (Figure 5d).
conductive filaments. When the filaments are connected to
both electrodes through the active layer, the conductivity of the
device is markedly increased, switching from high resistance 5.2. Charge Trapping
state (HRS) to low resistance state (LRS). By applying a further
reverse voltage bias, the metal atoms at the bottom will gradu- Charge trapping process is often caused by active materials
ally oxidize again into cations, and the conductive filaments will with charge trapping sites. With the applied external voltage
decompose, which decrease the device conductivity to its ini- bias, charge carriers will be gradually injected from the elec-
tial state, recovering from LRS to HRS. For instance, Khot et al. trode to charge trapping sites among the active film. When the
prepared a Ag/Ti3C2/Pt memristor, which utilized active Ag as voltage reaches a certain value, almost all the traps are filled
the top electrode and showed typical memristive characteris- with charge carriers. The accumulation of charges at the trap
tics (Figure 5a).[76] The working mechanism of Ag/Ti3C2/Pt is location helps to form a continuous charge transport pathway,
mainly ascribed to the electrochemical redox reaction of Ag and thus improving device conductivity and leading to the switch
the formation of conductive filaments in the Ti3C2 functional from HRS to LRS. Contrarily, by applying a reverse electric
layer (Figure 5b). field, the captured charge carriers can be released from the
Figure 5. a) Memristive characteristics of Ag/Ti3C2/Pt. b) Proposed ECM mechanism of Ag/Ti3C2/Pt. c) Memristive characteristics of Pt/Ti3C2/Pt.
d) Proposed VCM mechanism of Pt/Ti3C2/Pt. Reproduced with permission.[76] Copyright 2021, American Chemical Society.
trap centers, causing the conductive path to decompose. Thus, the potential of realizing multilevel memory performance,
the device reverts from the LRS to the original HRS, real- which hold promise to meet the demand of high-density data
izing bipolar switching behavior. Recent studies have revealed storage.[47] In addition, MXene-based memristors afford supe-
that MXenes,[47,48] carbon nanotubes,[148] metal nanoparticles rior merits of fast switching speed, simple device preparation,
(NPs),[149] and fullerenes[150] can serve as potential charge trap- low power consumption, and complementary metal oxide semi-
ping materials. conductor (CMOS) compatibility.[151] The memristors usually
One representative work was reported by Ding et al., who consist of two electrodes and a functional MXene layer between
prepared an Al/Ti3C2@ polyvinylpyrrolidone (PVPy)/indium- them, and can be switched between HRS and LRS under the
tin-oxide (ITO) memristor device with typical bipolar resis- external electric field. HRS can correspond to the low level
tive switching behavior (Figure 6a).[77] They fitted the current– (“0”) in the digital circuit and LRS can correspond to the high
voltage (I–V) curves with appropriate charge transport models, level (“1”) in the digital circuit. Therefore, the switch from HRS
indicating that the charge trapping process occurs during resis- to LRS is equivalent to the binary conversion from “0” to “1”
tive switching (Figure 6b). Figure 6c illustrates the charge trap- during data storage.[4,81,152,153]
ping mechanism of Al/Ti3C2@PVPy/ITO memristor. When the Zhang et al. first fabricated a MXene-based two-terminal
charge traps among Ti3C2 layer are filled, the conductive paths memristor, which adopted a laminated structure of Cu/Ti3C2/
(CPs) are formed, resulting in HRS to LRS transition. They SiO2/W (Figure 7a).[143] This memristor exhibited bipolar resis-
further utilized conductive atomic force microscopy (C-AFM) tive switching behavior under the voltage sweep from -2.5
measurement to examine the CPs between ITO and AFM tips to 2 V, with retention time over 1.0 × 103 s (Figure 7b). Wang
(Figure 6d). The C-AFM current mapping images indicate that et al. prepared a Ti3C2-ZnO composite and adopted it as the
the resistive switching behavior of Ti3C2-based memristor is active layer of ITO/Ti3C2Tx-ZnO/Al memristor, which showed
dominated by the formation and fracture of CPs (Figure 6e). In a high switching ratio and repeatable memristive charac-
addition, they adopted Kelvin probe force microscopy analysis teristics after 1.0 × 102 consecutive voltage scanning cycles
to verify the charge trapping and de-trapping processes under (Figure 7c).[140] Yan et al. reported a single-component MXene-
positive and negative voltage bias. based memristor of Al/Ti3C2Tx/Pt.[79] This memristor also dis-
played bipolar switching behavior, and retained stable even
after 3.0 × 102 voltage sweeping cycles (Figure 7d). No obvious
6. MXene-Based Memristor Applications degradation of LRS and HRS was observed after 1.0 × 106 cycles
and 1.0 × 105 s (Figure 7e,f). The high switching ratio and excel-
6.1. Data Storage lent endurance endow the memristor with great potential for
binary data storage. Mao et al. fabricated a memristor on the
MXene-based memristors can store data through the resistance basis of Ti3C2Tx quantum dots (Ti3C2TxQDs) with the structure
switching phenomenon, and several memristors have exhibited of Au/Ti3C2TxQDs@polyvinylpyrrolidone (PVP)/ITO, for which
Figure 6. a) Typical I–V curve of Al/Ti3C2@PVPy/ITO memristor device. b) Log-log plot of the memristor device at the SET process. c) The illustration
of the resistive switching mechanism based on charge trapping and CPs. d) The illustration of charge trapping and CP forming process between ITO
and AFM tip. e) 3D C-AFM current mapping images in i) read map (initial state, 0.4 V), ii) write map (4 V), iii) read map (0.4 V), iv) erase map (-6 V),
v) read map (0.4 V), and vi) random selected area from (iii); (i–v): 2.0 × 2.0 µm2, (vi): 2.0 × 2.0 nm2. Reproduced with permission.[77] Copyright 2019,
Royal Society of Chemistry.
PVP polymer was adopted to facilitate the film formation of LRS could be successfully implemented by adjusting the values
Ti3C2TxQDs via spin-coating.[147] The memristor device afforded of compliance currents (ICC), while retaining the bipolar resis-
reliable bipolar resistive switching behavior with an acceptable tive switching characteristics (Figure 8d). Moreover, the current
current ratio over 1.0 × 102 (Figure 7g), good retention ability over values and current distributions under different ICC indicated
1.2 × 104 s (Figure 7h), and narrow distributions of SET/RESET that these multistage resistive states were stable and distin-
voltages (Figure 7i). The Ti3C2TxQDs@PVP hybrid film exhibits guishable (Figure 8e,f). These results provide a reliable founda-
tunable memory and transient properties, which provide possi- tion for achieving MXene-based multilevel data storage.
bilities for implementing secure data storage application. Wang et al. prepared an Ag/V2C/W memristor, which
As shown in Figure 8a, Ding et al. took advantages of PVPy showed typical bipolar resistive switching behavior (Figure 9a).
polymer to fabricate Ti3C2-PVPy based memristor.[77] The device In addition, the device could afford multiple unidirectional LRS
could sustain for more than 1.0 × 103 cycles in the pulse test under different ICC (0.1, 0.5, 1, 5, 10, and 100 mA, Figure 9b),
mode, suggesting satisfactory endurance (Figure 8b). In addi- which could correspond to multilevel data storage (e.g., “1”,
tion, the statistic results of 50 devices showed narrow distribu- “2”, “3”, “4”, “5”, and “6”). Retention tests of these six resis-
tions of SET/RESET voltages (Figure 8c), indicating good sta- tive states revealed that the retention ability could be enhanced
bility and reproducibility. It has been documented that when under higher ICC (Figure 9c).[133] Generally, nonvolatile resistive
a material acquires more than two resistance states under memory can be classified into two types, i.e., write-once-read-
voltage stimuli, multilevel data storage (e.g., “0”, “1”, “2”, and many-times (WORM) memory and rewritable Flash memory.
“3”) can be achieved. Ding et al. also discovered that multiple Sun et al. reported a WORM-type MXene-based memory device
Figure 7. a) I–V characteristics of the Cu/Ti3C2/SiO2/W memristor device. b) Retention stability of different resistance states. Reproduced with permis-
sion.[143] Copyright 2019, Elsevier. c) I–V characteristics of the ITO/Ti3C2Tx-ZnO/Al memristor device. Reproduced with permission.[140] Copyright 2021,
Wiley-VCH. d) I–V characteristics of the Al/Ti3C2Tx/Pt memristor device. e) Endurance of the device. f) Retention stability of different resistance states.
Reproduced with permission.[79] Copyright 2019, Wiley-VCH. g) I–V characteristics of the ITO/Ti3C2TxQDs-PVP/Au memristor device. h) Retention stability
and current ratio of different resistance states. i) Statistic SET and RESET voltage distributions. Reproduced with permission.[147] Copyright 2019, Wiley-VCH.
(Figure 9d). Due to the free electrons among the skeleton of electronic components of the memristor are generally com-
MXenes, the surface engineering is feasible. Thus, Sun et al. posed of top/bottom electrodes and functional layer between
modified Ti3C2Tx by octylphosphonic acid and utilized the the two electrodes, which are very similar to the synaptic struc-
hybrid Ti3C2Tx-OP composite as the active material. The fabri- ture.[155–159] Functionally, the memristor can change resistance
cated device showed stable ternary resistive switching charac- by adjusting the migration of ions, which can simulate the
teristics (Figure 9e), with low SET voltages and good retention transmitting behavior of Ca2+ and Na+ ions in biological syn-
stability for more than 1.0 × 104 s (Figure 9f).[78] In the past few apses.[160–163] Therefore, memristors can be ideal candidates to
years, 2D MXene materials have aroused particular research mimic the dynamic behavior of synaptic neurotransmitters,
interests for resistive memory application, which afford which provide far-reaching significance for the development
appealing properties such as large switching ratio, long reten- of artificial neural networks. An essential feature of synapses
tion time, and excellent endurance. As shown in Table 2, the is plasticity. Synaptic plasticity mainly includes short-term syn-
recently reported MXene-based memristors with bipolar resis- aptic plasticity and long-term synaptic plasticity. Short-term
tive switching behavior are summarized. synaptic plasticity contains facilitation, short-term depression
(STD) and short-term potentiation (STP).[164–168] Paired-impulse
facilitation (PPF) is one typical feature of short-term synaptic
6.2. Artificial Synapses plasticity. PPF means that under the stimulation of a pair of
pulses, the intensity of the second conductance response
A synapse is a location where two neurons contact with each is greater than that of the first response, which is defined as
other and proceed information communication.[154] The PPF = (G2 − G1)/G1 × 100%, where G1 and G2 represent the
Figure 8. a) Schematic of Ti3C2-PVPy memristor device. b) Endurance of Ti3C2-PVPy memristor device. c) Statistic SET and RESET voltage distributions.
d) I–V characteristics of Ti3C2-PVPy memristor under different ICC of 0.1, 0.05, 0.01, 0.005, 0.0005, and 0.0001 A. e) Reversible resistance states over
60 cycles with various ICC (from left to right: 0.1, 0.05, 0.01, 0.005, 0.0005, and 0.0001 A). f) The distributions of LRS currents under different ICC (0.01,
0.005, 0.0005, 0.0001 A). Reproduced with permission.[77] Copyright 2019, Royal Society of Chemistry.
conductance response caused by the first and second input when applying a pair of pulses.[169,170] Long-term synaptic plas-
pulse respectively. Paired-impulse depression (PPD) is another ticity mainly displays in two aspects of long-term potentiation
feature of short-term synaptic plasticity, for which the intensity (LTP) and long-term depression (LTD). LTP denotes the rapid
of the second response is lower than that of the first response formation of long-term excitatory postsynaptic potential (EPSP)
Figure 9. a) I–V characteristics of the Ag/V2C/W memristor device under ICC of 10 mA. b) Typical positive I–V curves under different ICC of 0.1, 0.5,
1, 5, 10, and 100 mA. c) Retention stability for the Ag/V2C/W device after the positive stimulation with different ICC. Reproduced with permission.[133]
Copyright 2021, Elsevier. d) Schematic of the Al/Ti3C2Tx-OP/ITO device. e) I–V characteristics of the Al/Ti3C2Tx-OP/ITO device. f) Retention stability for
the Al/Ti3C2Tx-OP/ITO device. Reproduced with permission.[78] Copyright 2020, American Chemical Society.
Table 2. MXene-based memristors with bipolar resistive switching characteristics.
Top electrode Bottom electrode Materials Thickness Memristor characteristics Reference

LRS/HRS Retention Cycle VSET/VRESET
Ag W V2C 850 nm 104 2.0 × 103 s 100 5.0/-6.0 V [132]
Ag Pt Ti3C2/SiO2 50/80 nm 102 1.0 × 104 s 100 0.2/-0.2 V [142]
2
Au ITO Ti3C2TxQDs@PVP 100 nm 10 1.2 × 104 s 50 1.6/-2.9 V [147]
Al Pt Ti3C2Tx 150 nm 102 1.0 × 105 s 300 3.0/-2.0 V [79]
ITO Al Ti3C2Tx-ZnO 16 nm 104 1.0 × 104 s 100 -1.5/1.2 V [140]
Al ITO Ti3C2Tx@PVPy 35 nm 104 5.0 × 104 s 1000 0.6/-1.8 V [77]
5
Cu W Ti3C2/SiO2 2.22 µm/80 nm 10 1.0 × 103 s – 1.6/-1.0 V [143]
Au rGO Ti3C2Tx@PVP 80 nm 10 8.0 × 103 s 40 0.9/-1.8 V [146]
Cu W Ti3C2/SiO2 –/80 nm 10 3.0 × 103 s 800 0.7/-2.0 V [137]
TiN/Cu TiN Ti3C2/SiO2 –/80 nm 10 3.5 × 103 s 100 1.0/-1.0 V [144]
enhancement in postsynaptic neurons after presynaptic neu- Zhao et al. fabricated an artificial synaptic device with
rons receive repeatable stimulations, while LTD represents the oxidized MXenes as floating gate tunneling layer, SiO2 as
long-term reduction of synaptic transmission efficiency. Both dielectric layer and zinc tin oxide (ZTO) as channel layer
LTP and LTD processes are the basis of biological memory (Figure 11a).[181] Under the action of applying gate electrical
and learning activities, for which the synaptic weight can be pulses, the device could simulate typical biological synaptic
strengthened and/or weakened with time.[171–173] Spike-timing- behaviors. Figures 11b–d exhibited the excitatory post-synaptic
dependent plasticity (STDP) is a Hebbian synaptic learning current (EPSC) induced by 10 successive pulses with different
rule, which denotes the change of synaptic weight caused by amplitudes, widths and frequencies. With the increase of
the difference between presynaptic and postsynaptic spikes. pulse amplitude, pulse width, and pulse frequency, the higher
Another basic synaptic plasticity is called as spike-rate- EPSC responses were acquired. As shown in Figure 11e, the
dependent plasticity (SRDP), which is similar to STDP and red area represented the learning process, while the blue area
can modulate synapse weight by spike rate.[174–176] Traditional represented the forgetting process. By increasing the number
CMOS devices have been integrated to fabricate circuits for of pulses, it could be noted that the forgetting period in the
simulating synapses. However, such circuits are usually com- blue area became longer, which triggered the transition from
plex, which result in low processing efficiency and high energy short-term memory (STM) to long-term memory (LTM). This
consumption. In this regard, memristors have emerged as forgetting behavior is in line with Ebbinghaus forgetting law. In
promising contenders for artificial synaptic application.[177–179] addition to spontaneous forgetting, this device could also simu-
For memristors, the change of conductance during operation late the manual erasing process by applying multiple positive
can be utilized to emulate the change of synaptic weight (ΔW), presynaptic pulses. As illustrated in Figure 11f, the application
which is defined as ΔW = (Gpost − Gpre)/Gpre × 100%, where Gpre of consecutive positive pulses successfully accelerated the for-
and Gpost respectively represent the conductance of the mem- getting rate.
ristor in response to the presynaptic and postsynaptic pulses. Another work was conducted by Wang et al., which prepared
When Δt (i.e., tpost − tpre) and ΔW are both positive, the electrical an Ag/V2C/W memristor device (Figure 12a).[133] By adjusting
potentiation of memristor occurs. On the other hand, when Δt different ICC, the device exhibited two modes of threshold
and ΔW are both negative, the electrical depression of mem- switching and resistive switching. In a resistive switching
ristor appears.[133,180] mode, V2C-based memristor could mimic the influx and out-
Recently, Yan et al. reported a two-terminal memristor based flux behavior of Ca2+ in biological synapses. As shown in
on Ti3C2Tx, which could be used to simulate synaptic plas- Figure 12b, the response of conductivity induced by the second
ticity.[79] As shown in Figure 10a, the fabricated Al/Ti3C2Tx/Pt input pulse was greater than that induced by the first pulse,
device exhibited typical resistive switching behavior. Notably, suggesting PPF behavior. Figure 12c displayed the good fit-
the device presented an ultrafast response in pulse mode ting of PPF synaptic function with interval, which was attrib-
(Figure 10b), which succeeded to achieve electrical potentia- uted to the gradual accumulation of Ag ions and the formation
tion in conductance by applying a series of 20 consecutive posi- of more local conductive filaments. Figure 12d displayed the
tive pulses (2.0 V, 10 ns), and electrical depression in conduct- simulated STDP behavior of the memristor. The absolute value
ance followed by 20 consecutive negative pulses (-2.0 V, 10 ns). of ΔW decreased as Δt proceeded, indicating that the larger
They further examined the effects of different pulse duration spiking-time difference could lead to smaller synaptic weight
and amplitudes on the device conductance. As depicted in change, demonstrating the synaptic plasticity. In addition, this
Figure 10c,d, it was found that the conductance obviously memristor could be potentiated by high pulse frequency and
improved with the increase of pulse duration and amplitude, depressed by low frequency, which revealed the response to the
which manifested the tunable behavior of Ti3C2Tx-based mem- application of pulse frequency (Figure 12e). Figure 12f further
ristor for synaptic mimicking. displayed the change of conductance (in blue line) triggered
Figure 10. a) Schematic of the Al/Ti3C2Tx/Pt memristor device. b) The potentiation and depression curves of the Al/Ti3C2Tx/Pt memristor under the
application of successive alternating current (AC) pulses. A positive bidirectional pulse train is used to excite or inhibit the electronic synapses. c) Ini-
tial data of continuous pulse regulation with different pulse durations. d) Initial data of continuous pulse regulation with different pulse amplitudes.
Reproduced with permission.[79] Copyright 2019, Wiley-VCH.
by consecutive high frequency and low frequency pulses (in promise to afford superior data processing capability and
red line), which successfully emulated PPF and PPD synaptic implement biological scale simulation and calculation. Notice-
behaviors. Till now, a variety of MXenes have been reported ably, MXene-based memristors have shown extraordinary tal-
to achieve artificial synapses. As shown in Table 3, the recent ents in the field of neuromorphic computing.
representative MXene-based memristors for artificial synaptic The traditional computer systems widely adopt bistable
functions are summarized. circuits to perform binary computing (“0” and “1”).[5,184,185]
Although the binary computing is simple, its number of bits
is often too long. Compared with binary operation, the decimal
6.3. Neuromorphic Computing system has the base number of “10”, which is composed of “0”
to “9”.[186] The counting rule of decimal is every ten into one.
Nowadays, with the exponential growth of information, tra- In fact, the decimal arithmetic function has been involved into
ditional computer systems are confronted with the physical our life, which is promising for designing higher logic system
restrictions such as von Neumann architecture and memory beyond binary computing. Recently, Wang et al. doped 2D
wall.[178,182] Neuromorphic computing is emerging as a novel MXene of Ti3C2 with Ag nanoparticles and constructed an Al/
promising technology to address these issues, which has Ti3C2@Ag/Pt memristor (Figure 13a).[80] The device structure
increasingly aroused a lot of research attention. The neural is similar to biological synapse. It is worth noting that the Ag-
network in human brain can effectively handle complex tasks, doping strategy helps to overcome the problem of poor elec-
working as an ideal information processing system. In order trical performance caused by the dissolution of Ag electrode
to mimic the neural network, researchers are exploring novel under electrical field, and realize gradual bidirectional current
neuromorphic computing systems that can realize in-memory tuning instead of abrupt change in single-component Ti3C2-
processing.[183] The memristor-based artificial synapses hold based memristor (Figure 13b). Moreover, the decimal function
Figure 11. a) Schematic of the MXene-based artificial synaptic device. b) EPSC response to different gate pulse heights. c) EPSC response to different
gate pulse widths. d) EPSC response to different gate pulse frequencies. e) The device behavior changes from STM to LTM as the number of gate pulses
increases. f) LTP/LTD characteristics as a function of pulse numbers. Reproduced with permission.[181] Copyright 2021, Wiley-VCH.
of the device was achieved by calculating the percentage change the device reached 3.2 after 20 consecutive pulse stimulations
of initial to other stimuli current (PCC). The initial SET opera- (4.0 V, 1.0 ms). Therefore, when the PCC was counted to be 3.2,
tion was shown in Figure 13c, which revealed that the PCC of the number 20 would be counted in the next calculation. As
Figure 12. a) Schematic of the Ag/V2C/W memristor device. b) PPF behavior of the Ag/V2C/W memristor. c) The exponential fitting of PPF synaptic
function. d) STDP learning rules emulated by the Ag/V2C/W memristor. e) The conductivity response to different pulse frequencies. f) Experimental
demonstration of PPF and PPD synaptic behaviors under consecutive high frequency and low frequency pulses. Reproduced with permission.[133]
Copyright 2021, Elsevier.
Table 3. MXene-based memristors for artificial synaptic functions.
Memristors Voltage sweep range Synaptic functions Reference

PPF/PPD STP/STD LTP/LTD STDP/SRDP
Ag/V2C/W (-9.0 V to 9.0 V) Yes – – Yes [133]
Ag/V2C/TiO2/W (-0.6 V to 1.0 V) – – Yes – [138]
Ag/Ti3C2Tx/Pt (-10.0 V to 10.0 V) Yes Yes Yes – [135]
Al/Ti3C2Tx-ZnO/ITO (-1.0 V to 3.0 V) – – Yes – [140]
Cu/Ti3C2/SiO2/W (-2.4 V to 2.4 V) Yes – Yes – [136]
Al/Ti3C2/Pt (-3.0 V to 3.0 V) – – Yes Yes [76]
Al/Ti3C2@Ag/Pt (-0.2 V to 0.2 V) Yes Yes Yes – [80]
Ag/Ti3C2/SiO2/Pt (-1.0 V to 0.5 V) Yes Yes Yes – [142]
Al/Ti3C2Tx/Pt (-6.0 V to 6.0 V) Yes Yes Yes Yes [79]
displayed in Figure 13d, it was noted that the PCC of the device 6.4. Logic Circuits
also reached 3.2 after the addition of two series of 10 con-
secutive pulses, corresponding to the calculation processes of In addition to their outstanding performances in the fields of
10 + 10 = 20. The commutative law of addition was verified by data storage, artificial synapses, and neuromorphic computing,
A + B = B + A (5 + 15 = 15 + 5 = 20, Figures 13e,f). Intriguingly, MXene-based memristors have also shown attractive applica-
the commutative law of multiplication was also realized in this tion prospects in logic circuits.[18,47] A logic circuit is a circuit
memristor device, which was consistent with A × B = B × A that can perform logical operations, which usually contains
(4 × 5 = 5 × 4 = 20). As shown in Figures 13g,h, the multipli- several inputs and outputs.[187] When a certain logical relation-
cation of five groups with four positive pulses was identical ship between the input signals is satisfied, the logic circuit is
to the multiplication result of four groups with five positive turned on; otherwise, the circuit is turned off. The simple logic
pulses, acquiring the same PCC of 3.2. The decimal arithmetic circuits are usually composed of gate circuits, including NOT
operation of MXene-based memristor paves the way for imple- gate, AND gate, OR gate, NAND gate, NOR gate, XOR gate,
menting new conceptual neuromorphic computations. and XNOR gate.[188,189]
Recently, multimodal in-sensor computing has also been The development of integrated logic circuits confronts the
proposed to improve the working efficiency of artificial intelli- limitations of voltage loss and high energy consumption.[190–192]
gence systems. For instance, Wang et al. reported a multimodal Regarding this, researchers have discovered that the charge
Ti3C2-ZnO based memristor that combined visual data sensing, doping of 2D materials at the nanoscale holds promise to
relative humidity (RH) sensing, and pre-processing functions address the issues of integrated logic circuits. For example, Guo
to simulate the environmental adaptability of neuromorphic et al. fabricated a 2D MXene-based memristor by controlling
visual system.[140] For the in-sensor computing simulation, the oxidation time of MXene nanosheets and the doping of Ag
a single layer perception was built with 28 × 28 neurons (784 nanoparticles (Figure 15a).[83] This as-fabricated Ag nanoparti-
input neurons), 10 output neurons (10 classes from 0 to 9), and cles@MXene-TiO2 (namely as AMT) device exhibited bipolar
fully connected 784 × 10 synaptic weights (Figure 14a). Digital resistive switching behavior (Figure 15b), and could imple-
input pattern was sensed by the presynaptic neurons and trans- ment logic gate functions through the fine tuning of resist-
mitted as presynaptic spikes. Synaptic weight was controlled ance states under ultraviolet (UV) light radiation. The UV light
by humidity and light regulations, and then the postsynaptic radiation afforded a medium resistance state (MRS), which
neuron responded to the postsynaptic spikes to complete the was different from HRS and LRS under voltage bias. Thus, the
task of recognition and perception. Figure 14b displayed LTP multilevel data storage in a single AMT device was triggered
characteristics of the sensing memristor by 50 optical pulses (Figure 15c,d). The transitions among the three resistance
and LTD characteristics by 50 electrical pulses under different states could be achieved by the stimulation of electrical pulse
RH. It was found that the memristor showed more linear and UV light, as shown in Figure 15e. The input factors are
and symmetrical weight updating under 60% RH, resulting VSET, VRESET, and UV light, while the output factors are LRS,
in higher accuracy. In addition, the output images of Arabic HRS, and MRS.
numbers “1–9” after training under different RH levels mani- Compared with the conventional digital comparators that
fested that the artificial visual network training under 60% RH take up more area, time, and energy due to the integration of
condition could capture more objective features (Figure 14c). multiple logic gates, Guo et al. realized an efficient in-memory
Figure 14d showed the satisfactory recognition accuracies after magnitude comparator based on the fabricated multilevel photo
6.0 × 104 training cycles. These results indicate that the multi- electric AMT-based memristor.[81] The operation and principle
modal MXene-based sensing memristor can be applied for both of AMT-based comparators were shown in Figure 15f, where
low-level and high-level in-sensor computing, which provides the pulse voltages of Vp and Vq were regarded as two binary
the potential to develop intelligent neuromorphic visual system numbers (p and q). The initial state of the AMT-based com-
in device-level implementations. parator was set to MRS by UV light. Afterward, the Vp was
Figure 13. a) Typical I–V curve of the Al/Ti3C2@Ag/Pt memristor device. b) The asymptotic nonlinear I–V characteristics of the Al/Ti3C2@Ag/Pt mem-
ristor under consecutive positive and negative voltage stimuli. Demonstration of arithmetic computing with the Al/Ti3C2@Ag/Pt memristor: c) Initial
count. d) Addition. e,f) Commutative addition. g,h) Commutative multiplication. Reproduced with permission.[80] Copyright 2022, Elsevier.
applied on the top electrode, while the Vq was applied on the the resistance state (MRS), which is equivalent to the output
bottom electrode. When the pulse voltage of Vp or Vq is 0 V, p “010”. When p = 1 and q = 0, the voltage drop will set the resist-
or q is “0”. When the pulse voltage of Vp or Vq is a high voltage ance state to LRS, which induces the output “100”. Notably, the
of 3.0 V, p or q is “1”. Therefore, if Vp = 0 V and Vq = 3 V, this 4-bit AMT memristor-based comparators were also constructed,
input is equivalent to p = 0 and q = 1. According to the principle which could exponentially reduce the energy consumption
of AMT comparators, the voltage drop will reset the resistance during operation. As shown in Figure 15g, the 4-bit binary
state to HRS, which affords the output “001”. If p = q = 0 or numbers (A = A1A2A3A4 and B = B1B2B3B4) were first trans-
p = q = 1, the voltage drop on the device is 0 and will not alter formed to the equivalent voltage levels as input signals bit by
Figure 14. Real-time training for image recognition using the Al/Ti3C2-ZnO/ITO memristor device. a) Schematic of the high-level in-sensor computing
by employing the Al/Ti3C2-ZnO/ITO sensing memristor as a synapse to implement weight updating. b) RH-mediated plasticity of the sensing mem-
ristor showing LTP characteristics under the application of 50 optical pulses and LTD characteristics under the application of 50 electrical pulses.
c) Output images after 6.0 × 104 training epochs for the sensing memristor under different RH levels. d) Recognition rate as a function of RH levels.
Reproduced with permission.[140] Copyright 2021, Wiley-VCH.
bit. The four AMT memristors were initialized to MRS, where and SAED. In addition, the different types of MXene-based
the states of each memristor were obtained by the read voltage memristive materials and their typical switching mechanisms
to identify the magnitude of A and B. Two specific cases (A = B are summarized. The preparation and performance of different
and A ≠ B) with the relation between A and B were shown in memristor devices significantly depend on the physical and
Figures 15h–k, demonstrating the efficient logic operations of chemical properties of MXene materials. More importantly, the
such 4-bit AMT memristor-based comparators. It is noteworthy main text covers the applications of MXene-based memristors
that the input signals can be replaced by other functional sig- for data storage, artificial synapses, neuromorphic computing,
nals, and the number of bits can be reasonably extended. and logic circuits. The advances in these research not only
Since the digital comparator shares one conversion circuit, the show the great promise for implementing novel in-memory
overhead of the circuit does not increase with the number of computing technology using MXene-based memristors, but
bits. The digital comparator based on AMT opens up possibili- also open up opportunities of constructing artificial neural net-
ties for the future integrated functions of optoelectronic data work that can simulate the functionalities of human brain for
storage for simplified logic operations. It is believed that this human-level intelligence. Although tremendous progress has
study can promote the application of 2D MXenes in the field of been witnessed for MXene-based memristors, there still exist
optoelectronic cooperated logic circuits. several challenges that need to be considered and tackled.
First, the stable and reliable resistive switching performance
of memristors is very important for data storage and neuro-
7. Conclusion and Outlook morphic computing applications, which puts forward high
requirements for the efficient preparation of MXenes as well
In conclusion, this review provides a summary of recent pro- as their uniform films on substrates. However, through the
gress on 2D MXene-based materials for memristor applica- synthetic method of chemical etching, the obtained MXenes
tion. We briefly introduce two synthetic strategies of MXene may contain several defects. In addition, because of the active
materials. The “top-down” synthetic method is to selectively functional groups at the surface, the obtained MXenes are vul-
etch element A in MAX phase to obtain Mn+1Xn with appropriate nerable to oxygen and moisture in air condition, which can
reagents, while the “bottom-up” method uses CVD technology suppress the material longevity and device performance. The
to grow MXene film on substrate surface. Various chara- factors of oxygen, moisture, and heat should be taken into con-
terization methods of MXene materials are also enumerated, sideration during device preparation and operation. Therefore,
including Raman spectroscopy, XPS, SEM, AFM, XRD, TEM, the MXene-based memristors with long-term environmental
Figure 15. a) Schematic of the synthesis of Ag nanoparticles@MXene−TiO2 (AMT) material and the structure of the Au/AMT/ITO memristor device.
b) Typical I–V curves of the Au/MXene/ITO and Au/AMT/ITO devices. c) I–t curve of Au/AMT/ITO device under UV radiation. d) Retention stability
of the three states of LRS, MRS, and HRS. e) Operating input factors applied on the AMT-based device and resistance state transition under different
conditions. f) Operational principle of the AMT-based comparators. g) 4-bit binary numbers constructed by the AMT-based comparators. Experimental
results of equal conditions h) before and i) after the switching process. Experimental results of unequal conditions j) before and k) after the switching
process. Reproduced with permission.[81] Copyright 2021, American Chemical Society.
stability should be particularly focused on for further prac- satisfy both large-scale production and small-scale deposition
tical application. Moreover, the film-forming technique of control.
MXene-based memristors in laboratory mainly adopts spin- Second, compared with other 2D materials-based resistive
coating and post-annealing treatment. The solution-coated memories (e.g., graphene), MXene-based memristors remain at
films often suffer from inhomogeneous patches and/or disor- an early stage because of the short growth history of MXenes,
dered grain boundaries, which can impede the charge trans- which demand more research attention. Currently, most of the
port efficiency and degrade the device performance. Therefore, reported studies focus on the Ti3C2Tx materials. With the rapid
it is significant to develop a simple but efficient solution-pro- growth of MXene family, more MXene materials are anticipated
cessed technique and create a general principle for high- to be developed for memristor applications. In addition to the
quality MXene film preparation and device fabrication, which utilization of a single MXene material as memristive layer, it is
also worth developing MXene composites or heterostructures Overall, the progress of 2D MXene materials sheds light on
with other 2D materials for higher device performance. From the great potential in emerging optoelectronic and semicon-
the standpoint of structure, MXenes possess abundant surface ducting areas. Through addressing the scientific and technical
terminated functional groups, which provide opportunities issues, it can be anticipated that MXene-based memristors will
for assembling with other materials through appropriate sur- play a more and more important role for data storage, synaptic
face modification strategies, and inducing different memristor mimicking, neuromorphic computing, and logic operation.
device functions. In addition, the 2D planar plane and thin Taking the von Neumann bottleneck and memory wall of con-
thickness of MXenes endow them with high compatibility to ventional computer systems into consideration, the prospects of
other 2D materials via out-of-plane van der Waals interactions, in-memory computing and artificial neural network seem to be
which can achieve vertical layer-by-layer 2D heterostructures more fascinating. Despite the existing challenges to surmount,
for combining the intrinsic property of each 2D material. Thus, it is believed that the development and integration of MXene-
to integrate multi-functionalities into one MXene-based mem- based materials and memristors will provide positive possibili-
ristor device is another appealing direction. In fact, researchers ties for boosting new-generation information technology and
have been devoted to fabricating high-performance memristors artificial intelligent applications.
based on the doping of MXenes or the preparation of hetero-
structures. It is predictable that there will be more and more
diverse MXene functional materials for memristor applications Acknowledgements
in the future. Moreover, their ultra-thin thickness can facili-
Y.L. acknowledges financial support from the National Natural Science
tate the 3D stacking of MXene memristive layers, which is an
Foundation of China (Grants No. 22008164), the Natural Science
efficient way of realizing high-density device integration. The Foundation of Jiangsu Province (Grants No. BK20190939), the Natural
2D nanosheets of MXenes are also favorable for constructing Science Foundation of the Jiangsu Higher Education Institutions of
nano-devices, which hold great promise to implement minia- China (Grants No. 19KJB150018), and the foundation of Key Laboratory
turization of memristors for low-power consumption and fast of Synthetic and Biological Colloids, Ministry of Education, Jiangnan
respond speed. University (No. 1042050205225990/007). Q.Z. thanks the funding
Third, the practical application of MXene-based memristors support from City University of Hong Kong (9380117, 7005620, and
7020040) and Hong Kong Institute for Advanced Study, City University
for in-memory and neuromorphic computing is still a long way, of Hong Kong, Hong Kong, China. This work is also supported by the
which requires more cohesive cooperation than ever from the Natural Science Foundation of the Jiangsu Higher Education Institutions
theorists, physicists, chemists, material scientists, and com- of China (22KJB150037), Jiangsu Key Disciplines of the Fourteenth Five-
puter engineers. In terms of data storage, although the per- Year Plan (2021135), and the Suzhou Key Laboratory for Low Dimensional
formance of a single memristor can be greatly impressive in Optoelectronic Materials and Devices (SZS201611).
laboratory, the miniaturization and integration of the electrical
circuits still faces a challenge. The stability and reliability of
the devices under extreme environments (e.g., high tempera- Conflict of Interest
ture and high humidity) also need more investigation. In terms
The authors declare no conflict of interest.
of artificial synapses and neuromorphic computing, although
MXene-based memristors succeed to emulate the basic func-
tions of biological synapses, they lack sufficient capabilities to
completely realize the complex processing functions of human Keywords
brain. The simulation of actual synaptic functions through the 2D materials, data storage, logic operation, memristors, MXenes,
network of multiterminal synaptic devices requires more tech- neuromorphic computing
nical demonstrations. Currently, researchers attempt to imple-
ment the concept of artificial neural network by the combina- Received: July 20, 2022
Revised: October 3, 2022
tion of memristors and software algorithms. Nevertheless, due
Published online: November 14, 2022
to the existing restrictions of algorithms, research on artificial
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Songtao Ling is currently a graduate student at the school of Physical Science and Technology,
Suzhou University of Science and Technology. His main research interests focus on the prepara-
tion of 2D material-based memristors and their applications in data storage, artificial synapses,
and neuromorphic computing.
Cheng Zhang is currently a research fellow at the School of Physical Science and Technology,
Suzhou University of Science and Technology. He received his B.S. and Ph.D. degrees at the
College of Chemistry, Chemical Engineering and Materials Science, Soochow University. From
2019 to 2020, he joined Prof. Qichun Zhang’s group as a joint Ph.D. student. His research inter-
ests involve the synthesis and application of organic semiconductor materials, particularly organic
resistive memory devices.
Yang Li is currently an associate professor at the School of Physical Science and Technology,
Suzhou University of Science and Technology. From 2016 to 2017, he joined Prof. Qichun Zhang’s
group as a joint Ph.D. student. His research interests focus on the preparation of novel memris-
tive materials and devices and their applications for data storage and neuromorphic computing.
Qichun Zhang is a professor at the Department of Materials Science and Engineering, City
University of Hong Kong. Before he moved to Hong Kong, he was an associate professor with
tenure at the School of Materials Science and Engineering, Nanyang Technological University
of Singapore. He is currently a fellow of the Royal Society of Chemistry. His research interests
include rich-carbon conjugated materials and their applications for optoelectronic and semicon-
ductor devices (H-index: 101).

Adv Funct Materials - 2022 - Ling - Emerging MXene Based Memristors For in Memory Neuromorphic Computing and Logic

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Review

Emerging MXene-Based Memristors for In-Memory,

and predicted to reach ≈100 ZB by 2023.[1]

2.2. Bottom-Up a “bottom-up” method.[125–127] Due to the absence of oxygen-

Table 1. Different kinds of MXene-based memristive materials and their applications.

Functional layer Structure Application Reference

5.1. Filamentary Conduction 5.1.2. Valence Change Memory (VCM)

Table 2. MXene-based memristors with bipolar resistive switching characteristics.

Top electrode Bottom electrode Materials Thickness Memristor characteristics Reference

Table 3. MXene-based memristors for artificial synaptic functions.

Memristors Voltage sweep range Synaptic functions Reference

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