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Preparation and characterization of anhydrous magnesium carbonate: Effect

of different anions of the magnesium sources

Xuepu Cao, Ruilei Zhang, Hua Zhao, Runjing Liu

PII: S0022-0248(24)00018-6
DOI: https://doi.org/10.1016/j.jcrysgro.2024.127583
Reference: CRYS 127583

To appear in: Journal of Crystal Growth

Received Date: 16 November 2022

Revised Date: 8 March 2023
Accepted Date: 10 January 2024

Please cite this article as: X. Cao, R. Zhang, H. Zhao, R. Liu, Preparation and characterization of anhydrous
magnesium carbonate: Effect of different anions of the magnesium sources, Journal of Crystal Growth (2024),
doi: https://doi.org/10.1016/j.jcrysgro.2024.127583

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 Preparation and characterization of anhydrous magnesium

carbonate: Effect of different anions of the magnesium sources

Xuepu Caoa, Ruilei Zhanga, Hua Zhaoa, Runjing Liua,*

aCollege of Chemical and Pharmaceutical, Hebei University of Science & Technology,

Shijiazhuang 050018, Hebei province, PR China

*Corresponding author. Email addresses: liurj@hebust.edu.cn (Runjing Liu)

Abstract：The hydrothermal synthesis process for anhydrous magnesium carbonate

(MgCO3) from Na2CO3 and three different soluble magnesium sources (MgSO4, MgCl2
and Mg(NO3)2) are investigated. High purity MgCO3 particles are synthesized at the
reaction temperature of 160 ℃, the reaction time of 6 h, and the reactant ratio of 1:1 in
the three groups of experiments. The effect of different anions of the magnesium
sources are investigated through comparison of the morphologies and specific surface
areas of the obtained MgCO3 particles. MgCO3 particles using Mg(NO3)2 as the
magnesium source shows the thinnest layers stacked structure with flawless surface and
the least specific surface area. Besides, the PHREEQCI computation results show that
the water activity of the reaction solution using Mg(NO3)2 as the magnesium source is
the lowest. Based on the above results, the possible synthesis mechanism of MgCO3
with the different magnesium sources are proposed.

Keywords: A1. Anhydrous magnesium carbonate; B1. Different magnesium sources;

C1. Comparison; D1. Synthesis mechanism

1. Introduction

Anhydrous magnesium carbonate (MgCO3) is a high value-added inorganic

functional material due to its low solubility, high chemical and thermodynamic stability
properties. It has been widely used as additives of polyvinyl chloride (PVC) for higher
mechanical and flame retardant properties [1, 2], semi-coke for reducing the emissions
of SO2 and NOx [3], molybdenite concentrate for oxidizing roasting improvement [4],
optical materials [5], flame retardants [6], and many other industrial areas [7, 8].

Stimulated by the above applications, many synthesis methods, mainly including

hydrothermal synthesis [1, 2, 5, 9-12], solvothermal synthesis [13], solid reaction [14]
and precipitation [15], were developed. Among them, the hydrothermal carbonization
method is more often used as the high-temperature conditions are favorable for
accelerating the reaction and the synthesized products usually have regular shape, high
purity, and less agglomeration [1]. Zhao et al. [1] hydrothermally synthesized MgCO3
from urea and MgSO4 with different crystal modifiers. Bi et al. [2] prepared MgCO3
from urea and MgCl2 using sodium dodecylbenzene sulfonate as the crystal direction
agent. Ni et al.[5] synthesized MgCO3 from hexamethylenetetramine and magnesium
acetate by the addition of a certain amount of sodium sulfate. Lu et al. [9] synthesized
MgCO3 using MgSO4 as magnesium source and ascorbic acid as both CO2 source and
crystal modifier. Sandengen et al. [10] synthesized MgCO3 from hydromagnesite and
CO2 using monoethylene glycol to decrease the water activity and avoid the hydrate
phases of magnesium carbonate. Xing et al. [11] synthesized MgCO3 from urea and
various magnesium sources. Dong et al. [12] prepared MgCO3 under the present of
potassium ions solution.

However, most of the above studies using hydrothermal synthesis method

introduced various additives, which were not economical in synthesis and post-
treatment process. And beyond that, they took no account of the effects of different
anions of magnesium source on the MgCO3 formation process, but which may have
great influence on the morphology of the products.

Our previous work has shown that the different ions can affect morphology of the
magnesium salts [16], and the surface roughness directly affects the purification process.
Therefore, for high purity products, the smoothness of the samples become very
important. It is necessary to investigate the effect of different anions of the magnesium
sources on morphology of MgCO3, although the its impact may be subtle compared
with other factors including temperature, time, stoichiometric ratio.

It is generally known that, high-quality and high-purity MgCO3 particles are

difficult to prepare under mild conditions, which mainly because the Mg-cation has a
highly ionic character and possesses strongly bonded layers of water dipoles [17]. So,
[Mg(H2O)6]2+ complexes are dominant in aqueous solution. The dehydration process
of the ions is determined by their chemical nature, ionic radii, charge, water activity,
etc. The decrease in water activity can stimulate the dehydration process [18]. When
2
the CO2 source is added to the reaction system, the CO3 can prompt the dehydration
process of [Mg(H2O)6]2+ complexes. But meanwhile, it must compete with the anions
2
from the magnesium source. The competitiveness of these anions relative to CO3 can
have an important influence on the MgCO3 formation process.

Therefore, we mainly investigated the effect of different anions of the magnesium

sources on synthesis of MgCO3. The experiments were carried out through the
hydrothermal method using Na2CO3 and magnesium sources (MgSO4, MgCl2 and
Mg(NO3)2 from industrial magnesium sources [19-21]) as reactants. There was only
one step to get the final product without additives. Firstly, we investigated the effect of
the reaction temperature, time, and the ratio of the reactants on the final product. Then,
the morphologies and specific surface areas of the different MgCO3 products were
compared, and the water activity of the reaction solution were calculated by
PHREEQCI program. Finally, the possible synthesis mechanism of MgCO3 with the
different magnesium sources were discussed.

2. Materials and methods

2.1 Materials

Magnesium chloride (MgCl2·6H2O), magnesium nitrate (Mg(NO3)2), magnesium

sulfate (MgSO4·7H2O) and sodium carbonate (Na2CO3) (analytical grade, Tianjin
Yongda Chemical Reagent Company, Tianjin, China) were used as received without
further purification. Deionized (DI) water was prepared in the lab and used in all
procedures.

2.2 Experimental unit

In this work, three different kinds of soluble magnesium salts including MgCl2,
Mg(NO3)2 and MgSO4·were used as the magnesium source. Na2CO3 was used as the
precipitant. As shown in Fig. 1, we firstly prepared a certain amount of 2 mol/L
magnesium salt solution in (1) beaker. Na2CO3 was directly added to the solution
according to the given reactant ratio. The slurry was mixed fully about 1 h, then
transferred to (2) polytetrafluoroethylene sleeve protected by (3) crystallization kettle,
finally heated in (4) rotary furnace at the given temperature with a certain time. After
cooling, filtering, washing, drying steps, the desired product was obtained. The
experimental conditions for MgCO3 synthesis in this work are shown in Table 1.

Fig. 1 Experiment setup of MgCO3 production. (1) Na2CO3 solution; (2) peristaltic pump; (3)
stirrer; (4) Mg2+ solution; (5) water bath; (6) Polytetrafluoroethylene sleeve; (7) Crystallization
kettle; (8) Rotary furnace; (9) Motor; (10) Controller.

Table 1 Summary of experimental conditions for MgCO3 synthesis

Reaction time Reaction temperature Reactant ratio

Exp. magnesium source
(h) (℃) (mol(Mg2+)/mol(Na2CO3))
 A1 MgSO4 4, 6, 8 160 1:1

A2 MgSO4 6 130, 140,150,160 1:1

A3 MgSO4 6 160 1:0.9, 1:1, 1:1.6, 1:2

B MgCl2 6 160 1:1

C Mg(NO3)2 6 160 1:1

D1 MgSO4 5 160 1:1

D2 MgCl2 5 160 1:1

D3 Mg(NO3)2 5 160 1:1

2.3 Measurement methods

X-ray powder diffraction (XRD) patterns of the samples were taken by employing
a Rigaku D/max-2500X-ray diffractometer (Rigaku, Japan). The morphologies of the
samples were investigated by using scanning electron microscope (SEM) (S4800-Ⅰ,
HITACHI, Japan). Thermogravimetric analysis-differential scanning calorimetry (TG-
DSC) (STD-2960, TA USA) was used to quantify the composition of the sample. The
surface areas of the samples were analyzed by Brunauer–Emmett–Teller–Barrett–
Joyner–Halenda (BET-BJH) (Quantachrome, USA). The PHREEQCI program
(version 3.7.3) was used for simulation of the MgCO3 synthesis process. The LLNL
model was selected.

3. Results and discussion

3.1 Synthesis of MgCO3 using MgSO4 as the magnesium source

3.1.1 Effect of reaction time

The effect of reaction time on the synthesis of MgCO3 particles was investigated
in this section, corresponding to the Exp. A1 in Table 1. The TG results of MgCO3
prepared at different reaction time are shown in Fig. 2. Fig. 2a shows that, when the
reaction time is 4 h, the TG curve of the sample is similar to that of basic magnesium
carbonate [22], which includes dehydration, dihydroxylation, and decarbonation
process. When the temperature is below 200 ℃, the small mass loss is expected to be
due to the desorption of physically adsorbed water. In the temperature range 200 ℃ ~
400 ℃, the mass loss is expected to be due to either dehydration or dehydroxylation,
or both. when the temperature is above 400 ℃, the mass loss is expected to be due to
decarbonation. The total weight loss rate of the sample is about 59.14 %, indicating the
obtained sample consists of a large amount of hydrated basic magnesium carbonate and
a small amount of anhydrous magnesium carbonate.

As shown in Fig. 2b, when the reaction time is prolonged to 6 h, the weight loss
stage is at around 500 ℃ ~ 600 ℃ and the residue weight at 700 ℃ is 47.6 %, which
equals to the theoretical value of 47.6 % of MgCO3, indicating that the obtained sample
has the high probability of the pure MgCO3 particles. When the reaction time is
prolonged to 8 h as shown in Fig. 2c, the weight loss curve of the sample is similar to
that of 6 h, therefore, the reaction time is selected 6 h.

100
(b)
90
(a)
(c)
Weight change (%)

80

70

60
(a) 4 h
(b) 6 h
50
(c) 8 h

40

100 200 300 400 500 600 700

Temperature (C)

Fig. 2 TG results of MgCO3 prepared at different reaction time with MgSO4 as the magnesium
source, the reaction temperature of 160 ℃, and the material ratio of 1:1

In order to validate the above statements, XRD patterns of the samples prepared
at different reaction time were measured. The results are shown in Fig. 3. Fig. 3a shows
the XRD profile of the product obtained at 4 h corresponding to the sample in Fig. 2a.
The 2θ reflections of the sample match the characteristic peaks of MgCO3 and
4MgCO3·Mg(OH)2·4H2O [12], which indicting the sample is the co-precipitate of the
foregoing two substances. But the diffraction peaks of MgCO3 at 32° and 43° are
extremely weak, indicating that the amount of MgCO3 in the sample is very small.
 Fig. 3b and Fig. 3c show the XRD profiles of products obtained at 6 h and 8 h
respectively. The 2θ reflections of the samples are in good agreement with the reported
data for MgCO3 in the literatures [12]. No characteristic peaks of other impurities are
observed for both samples, which indicate that the obtained products are of high purity.
In addition, the intensive XRD peaks show that they both possess good crystallinity.

★
(c) 8 h
★
★
★ ★

★
(b) 6 h
Intensity(a.u.)

★
★ ★

◆
◆ (a) 4 h

◆ ◆ ◆ ◆
◆◆ ◆ ◆ ◆ ◆
★
★

standard pattern of Hydromagnesite

standard pattern of Magnesite

10 20 30 40 50 60
2θ ()

Fig. 3 XRD results of MgCO3 prepared at different reaction time with MgSO4 as the magnesium
source, the reaction temperature of 160 ℃, and the reactant ratio of 1:1 (★: MgCO3; ◆:
hydromagnesite (4MgCO3·Mg(OH)2·4H2O))

3.1.2 Effect of reaction temperature

The effect of reaction temperature on the synthesis of MgCO3 particles was

investigated, corresponding to the Exp. A2 in Table 1. The TG results of MgCO3
prepared at different reaction temperature are shown in Fig. 4. Fig. 4a shows that, when
the reaction temperature is 130 ℃, the TG curve is similar to that in Fig. 2a, and the
total weight loss rate of the sample is about 53 %, which indicates the sample is the co-
precipitate of MgCO3 and 4MgCO3·Mg(OH)2·4H2O [23]. When the reaction
temperature is increased above 140 ℃ ~ 150 ℃ as shown in Fig. 4b and Fig. 4c, there
is a obvious weight loss of the sample below 500 ℃, indicating the samples still contain
a small amount of 4MgCO3·Mg(OH)2·4H2O. When the reaction temperature is
increased above 160 ℃ as shown in Fig. 4d (same to Fig. 2b), there is only a sharply
weight loss above 500℃, indicating that the sample is pure MgCO3.

When the reaction temperature is lower, Mg2+ firstly transforms into basic
magnesium carbonate due to the high hydrous features of Mg2+. When the reaction
temperature is increased, the hydration properties of Mg2+ has subsided, resulting in the
decrease of the proportion of basic magnesium carbonate and increase of that of
anhydrous magnesium carbonate of the sample. When the reaction temperature
continues to increase, the sample are completely converted to anhydrous magnesium
carbonate. Therefore, the increase in reaction temperature is conducive to the formation
of anhydrous magnesium carbonate, the reaction temperature is selected 160 ℃.

100

(d)
90

(a)
80
Mass (%)

70 (a)130℃
(b)140℃ (b)
(c)150℃
60 (c)
(d)160℃

50

40
0 100 200 300 400 500 600 700

Temperature (C)

Fig. 4 TG results of MgCO3 prepared at different reaction temperature with MgSO4 as the
magnesium source, the reaction time of 6 h, and the material ratio of 1:1

3.1.3 Effect of reactant ratio

The effect of the reactant ratio on the synthesis of MgCO3 particles was
investigated, corresponding to the Exp. A3 in Table 1. The TG results of MgCO3
prepared at different reactant ratios are shown in Fig. 5. As shown in Fig. 5a, when the
molar ratio of magnesium sulfate to sodium carbonate is 1:0.9, the TG curve is similar
to that in Fig. 2b, which indicates the high purity of the as-obtained MgCO3. When the
reactant ratio is 1:1, the TG curve shown in Fig. 5b is same to that in Fig. 2b. When the
molar ratio is 1:1.6 or 1:2, the residue weight of the samples at 650 ℃ is 66.7 % and
75.3 % respectively as shown in Fig. 5c and Fig. 5d, which are much higher than the
theoretical value of the pure MgCO3, indicating the as-obtained samples maybe the
mixture of MgCO3 and other substance.
 100

90 (a)

(b)
80 (a) 1:0.9
Weight change (%)

(d)
(b) 1:1
70 (c) 1:1.6
(c)
(d) 1:2

60

50

40
100 200 300 400 500 600 700

Temperature (C)

Fig. 5 TG results of MgCO3 prepared at different reactant ratio with MgSO4 as the magnesium
source, the reaction time of 6 h, and the reaction temperature of 160 ℃

In order to identify the composition of the mixture, the samples obtained at the
molar ratio of 1:1.6 and 1:2 were charactered by XRD. The results are shown in Fig. 6.
As shown in Fig. 6c and Fig. 6d, the samples obtained at the reactant ratio of 1:1.6 and
1:2 are the mixture of MgCO3 and MgCO3 ▪ Na2CO3. And, the content of MgCO3 ▪
Na2CO3 in the sample is increased with the increase of the proportion of Na2CO3.
Therefore, the reactant ratio of 1:1 is selected.
 ◆
(d)1：2.0
★
★ ◆ ◆ ◆◆
◆
★ ◆ ◆ ◆◆
★
★ (c)1：1.6
★
Intensity(a.u.)

◆★ ★ ★
★
★ (b)1：1.0
★
★★ ★
★
★ (a)1：0.9
★
★★ ★
★

20 30 40 50 60 70 80
2θ(°)

Fig. 6 XRD profiles of MgCO3 obtained at the molar ratio of (a) 1:0.9, (b) 1:1.0, (c) 1:1.6 and (d)
1:2 with MgSO4 as the magnesium source, the reaction time of 6 h, and the reaction temperature
of 160 ℃ (★: MgCO3; ◆: MgCO3 ▪ Na2CO3)

3.2 Effect of different anions on synthesis of MgCO3

3.2.1 Experimental comparison

In this section, the effect of the different magnesium salts on synthesis of MgCO3
were investigated. We performed additionally two experiments for MgCl2 and
Mg(NO3)2 corresponding to Exps. B and C respectively in Table 1. XRD results of
MgCO3 prepared using MgCl2 and Mg(NO3)2 as the magnesium sources at the reaction
temperature of 160 ℃, the reaction time of 6 h, and the reactant ratio of 1:1 are shown
in Fig. 7. The results indicate that both products are high purity MgCO3.
 ★
（a）

Intensity(a.u.) ★

★ ★

★
（b）

★
★ ★

10 20 30 40 50 60
2θ (degrees)

Fig. 7 XRD results of MgCO3 prepared using (a) MgCl2 and (b) Mg(NO3)2 as the magnesium
source at the reaction temperature of 160 ℃, the reaction time of 6 h, and the reactant ratio of 1:1
(★: MgCO3)

Fig. 8 shows the SEM images of MgCO3 produced by different magnesium salts
MgSO4, MgCl2, and Mg(NO3)2 at the optimal conditions. Fig. 8a and Fig. 8b show that
the MgCO3 particles using MgSO4 as the magnesium source are the sheet stacked cubes
with particle size in the range of 1 μm ~ 10 μm. And, there are many crystal defects on
the surface of the particles. Figs. 8c and Fig. 8d show that the MgCO3 particles using
MgCl2 as the magnesium source are also the sheet stacked cubes with particle size in
the range of 3 μm ~ 10 μm. However, the crystal defects on the surface are less and the
crystalline layers of the particle are thinner than that of MgCO3 particles using MgSO4
as the magnesium source. When using Mg(NO3)2 as the magnesium source, the
obtained MgCO3 particles are also the sheet stacked cubes with particle size in the range
of 3 μm ~ 10 μm as shown in Fig. 8e and Fig. 8f. However, the surfaces of the particles
are almost flawless, and all the crystalline layers of each particle are the thinnest
compared with the previous two particles.
Fig. 8 SEM images of MgCO3 produced by different magnesium salts (a) MgSO4; (b) the
corresponding high magnification image of (a); (c) MgCl2; (d) the corresponding high magnification
image of (c); (e) Mg(NO3)2; (f) the corresponding high magnification image of (e), at the reaction
temperature of 160 ℃, the reaction time of 6 h, and the reactant ratio of 1:1

Table 2 shows that the specific surface area of MgCO3 particles using MgSO4 as
the magnesium source is largest among the samples. While, MgCO3 particles using
Mg(NO3)2 as the magnesium source is smallest. This is probably because that the large
particle size and smooth surface reduce the specific surface area of MgCO3 particles
using Mg(NO3)2 as the magnesium source, which is consistent with the results shown
in Fig. 8.

Table 2 BET surface area of MgCO3 produced by different magnesium salts

Base solution Specific surface area of MgCO3 (m2/g)

MgSO4 99.30

MgCl2
68.86

66.47
Mg(NO3)2

In addition, we investigated the reaction process for all the three magnesium salts
at the reaction temperature of 160 ℃, the reaction time of 5 h, and the reactant ratio of
1:1, corresponding to Exps. D1-D3 in Table 1. The results are shown in Fig. 9.

100

90
(a)
Weight change(%)

80 (b)
2-
(a) SO4
70 (b) Cl- (c)
(c) NO3-
60

50

40
0 100 200 300 400 500 600 700 800
Temperature(℃)

Fig.9 TG results of MgCO3 produced by different magnesium salts with the reaction time of 5 h,
the reaction temperature of 160 ℃ and the material ratio of 1:1

Fig. 9a is the TG result of the sample prepared with SO42- solution, which has a
weight loss of approximately 23.81 % in the range of 500-600 °C and approximately
29.43 % below 500 °C, indicating that there is a large amount of basic magnesium
carbonate in the sample. Fig. 9b shows the reaction result with Cl- solution. The weight
loss of the sample in the range of 500-600 °C is about 46.28 %, and the weight loss
below 500 °C is small, which indicates that there is still a small amount of basic
magnesium carbonate in the sample. Compared with MgSO4, MgCl+ is a weakly
associated complex [24], which is beneficial for CO32 competition. The TG result of

the sample prepared in NO3-solution is shown in Fig. 9c. The sample only occurs
weightlessness in the range of 500-600 °C and the weight loss rate is about 51.24 %
which indicates that most of the sample have been converted to MgCO3. The TG results
shown in Fig. 9 indicate that ionic strength had a strongly positive effect on the reaction
rate during the MgCO3 crystallization period [25].

3.2.2 Mechanism of MgCO3 preparation by different magnesium salts

The difficulty in precipitating the anhydrous magnesium carbonate is often

attributed to the highly hydrated character of Mg2+ in solution. [Mg(H2O)6]2+
complexes is predominant in the reaction solution. Therefore, reducing the energy
barrier of dehydration of [Mg(H2O)6]2+ complexes is necessary for anhydrous
magnesium carbonate formation.

In this paper, we mainly investigated the effect of different anions of the

magnesium sources on synthesis of anhydrous magnesium carbonate. Therefore, the
following analysis was performed with other reaction conditions consistent.

When the reactant Na2CO3 is added to the reaction solution, the CO32 competes

with the SO 24 , Cl , or NO3 (from different magnesium sources) and H2O existing

in the solution [18]. The radius of SO 24 is biggest, then, NO3 and Cl in turn.

Therefore, compared with NO3 and Cl , SO 24 maybe more conducive for

dehydration of [Mg(H2O)6]2+. However, the concentration of NO3 and Cl is twice

that of SO 24 with the same amount of magnesium source according to their chemical

formulas. Thus, the ionic strength of NO3 solution is higher than that of SO 24 . Based

on the analysis above, using Mg(NO3)2 as the magnesium source is most conducive for
dehydration of [Mg(H2O)6]2+, which is consistent with the results shown in Fig. 9.
 1.0

0.9

Water activity of the solution

0.873
0.851
0.827
0.8

0.7

0.6

0.5
MgSO4 MgCl2 Mg(NO3)2

Fig. 10 Water activity of the solution with different magnesium salts

In order to validate the above statements, we calculated the water activity of the
three reaction solutions. As shown in Fig. 10, MgCO3 using Mg(NO3)2 as the
magnesium source shows the lowest water activity which can be the result of bigger
ionic radius and higher ionic concentration of NO3 . Lower water activity favors the

ion dehydration processes and, hence, the decrease of the [Mg(H2O)6]2+ complexes in
the saturated solutions. Therefore, the decrease in water activity can stimulate the
formation of MgCO3. The possible mechanism of the effect of the different anions of
the magnesium sources on MgCO3 preparation is shown in Fig. 11.
 Fig. 11 Mechanism of the effect of different anions of the magnesium sources on MgCO3
preparation

4. Conclusions

In this work, we synthesized the MgCO3 from Na2CO3 and three different
magnesium sources (MgSO4, MgCl2 and Mg(NO3)2). We obtained the reaction
condition for the high purity MgCO3 particles. It should be noted that MgCO3 ▪ Na2CO3
can be synthesized when the reactant ratio of Mg2+ and Na2CO3 is less than 1. The
morphologies and specific surface areas of the MgCO3 particles using MgSO4, MgCl2
and Mg(NO3)2 respectively as the magnesium sources are different. MgCO3 particles
using Mg(NO3)2 as the magnesium source shows the thinnest layers stacked structure
with flawless surface and the lowest specific surface area. We used the PHREEQCI
program to calculate the water activity of the reaction solutions. Larger ionic radius and
higher anion concentration are conducive for dehydration of [Mg(H2O)6]2+, and
consequently stimulate the formation of MgCO3. Based on the above results, the
possible synthesis mechanism with different anions of the magnesium sources were
proposed, which can help the researches to understand the crystal growth process of
MgCO3.

Acknowledgments

Hebei Natural Science Foundation [Grant B2021208026] and Open Foundation of

State Key Laboratory of Chemical Engineering [No. SKL-ChE-21B02] are
acknowledged.
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The effect of different anions of the magnesium sources on MgCO3 synthesis are
investigated.

The morphologies and specific surface areas of the MgCO3 are characterized.

The water activity are calculated.

The possible synthesis mechanism is proposed.

 CRediT authorship contribution statement

Xuepu Cao: Conceptualization, Methodology, Software, Writing-original draft.

Hua Zhao: Data curation.

Ruilei Zhang: Writing - review & editing, Validation, Visualization, Investigation.

Runjing Liu: Supervision.

Declaration of interests

☒ The authors declare that they have no known competing financial interests or personal
relationships that could have appeared to influence the work reported in this paper.

☐The authors declare the following financial interests/personal relationships which

may be considered as potential competing interests: