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    of 11
    us) United States 2) Patent Application Publication co) Pub. No.: US 2020/0239401 A1 oy ow 0) a @ (86) 6) LIU et al. METHOD FOR DIRECTLY PRODUCIN METHYL ACETATE ANDIOR ACETIC ACID FROM SYNGAS, Applicant: DALIAN INSTITUTE OF (CHEMICAL PHYSICS, CHINESE ACADEMY OF SCIENCES, Dalian om Inventors: Hongchso LIU, Dalian (CN) Wenllang ZHU, Dalian (CN): ‘hongmin LIV, Dalian (CN): Yous LIU, Dalian (CN): Shiping LIU, Dalian (CN); Full WEN, Dalian (CN) ‘Youming NI, Dalian (CN) MA, Dalian (CN) Assignee: DALIAN INSTITUTE OF (CHEMICAL PHYSICS, CHINESE ACADEMY OF SCIENCES, Dalian om Appl. Nos 161647,174 PCT Filed: Sep. 29, 2017 PCE No: PETICN2017/104609 § 371 (XI), (@) Date: Mar. 13, 2020 Publication Classification core 6736 care S110 (2006.01) (2006.01) US 202002394011 (43) Pub. Date: Jul. 30, 2020 ors 804 200501) BOL 806 (2006.01), BOLI 237889 (200501), BOL 2300 (2006.01), BOL 29/40 (200501), BOL 2918 (2006.01), BOIS 29/70 (200501) CO7C 6736 (2013.01); CO7C S10 (2013.01); Bord 870492 (2013.01); BOLT 8/065 (2013.01); BOLT 2378892 (2013.01) ‘BOL! 2208/025 (2013.01), BOLT 29/40 (2013.01); BOL 298 (2013.01); BOLT 29/70 (013.01); BOLI 29/7023 2013.01); BOLT 21002 (201301), ABSTRACT on method for directly prodncing methyl acetate andor acetic ‘acid from syngas, carried out in atleast two reaction zones, including: feeing a raw material containing syngas into a First reaction zane to contact and reat With metal catalyst Allowing an obtained effluent to enter a second reaction zone ‘irelly oF after the ation of carbon monoxide 50 a8 10 contact and react with a solid acid catalyst; separating the bined efluent to obtain product of acetate andlor acetic ‘cid, and optionally returning a residual pan to enter the first reaction Zone and/or the second reaction zone to recycle the reaction. This provides a novel method for dtectly convert ing syngos into methyl acetate andlor acetic acid. Further, the product selectivity of the product of methyl acetate oF acetie aeid is greater than 93%, and the quantity of methyl foetate and acetic acid may be adjusted according t0 pro- essing Patent Application Publication Jul. 30, 2020 Sheet 1 of 2 US 2020/0239401 AI Methyl acetate and/or Acetic acid FIG. 1 Patent Application Publication Jul. 30,2020 Sheet 2 of 2. US 2020/0239401 Al Methyl acetate and/or Acetic acid FIG. 2 US 2020/0239401 AI METHOD FOR DIRECTLY PRODUCING METHYL ACETATE ANDIOR ACETIC ACID FROM SYNGAS. TECHNICAL FIELD. 10001] The present invention relates to a method for directly converting syngas to prodice methyl acetate andor ‘acetic acid BACKGROUND 10002} Methyl acetate is a colorless, scented liguid with less toxicity and. sirong dissolving ability, which is un ‘excellent cellosolve and spray solveat. Ax an important intermediate in the chemical industry, methyl acetate cua produce downstream products including ethanol, acetic acid, ‘acetic anhydride, methyl acrylate, vinyl acetate, and ace amide, ete, and have a very broad application prospect. [0003] Acetic acid is an important onganie acid, whieh ean be used ia the production of vinyl acetate, acatic anhydride, cellulose acctate, acetates and metal accttes. Acetic acid is ‘also used as a solvent and raw material in pesticides, Pharmaceuticals and dyes and other industries, Acetic acids ‘widely used in pharmaceutical manufacturing, textile print- ing and rubber industries [0003] Ac present, the main synthesis methods of methyl soctate are: reactive distillation of methanol and acctic acid as raw materials; methanol dehydrogenation synthesis of ‘ethanol as raw material; one-step methane casboylatio method of methanol and CO as ra materials; homologatis ‘of methy] formate and dimethyl ether carbonylation. The industrial produetion method of acetic seid is mainly care bonylation of methanol on Rh-T or Ir—I satalyst to gen- ‘erate acetic acid, Because this process uses precious metal fetalysts, and there is also the production of hydrogen halide, the requirements for production equipment are ‘extremely high, [0005] The production of «large variety of basic chemical raw materials and high value-added fine chemicals using syngas a¢ raw materials has been hot topic in the Held of Cctalyss. The direet prepartion of ethanol from syngas is 3 new process for etlanol preparation in recent years. From the point of view of process and cost, the process of direst preparation of ethanol from syngas is short, the operating ‘ost i relatively exonomieal, and the investment cost slow. However, ftom the perspective of thermodynamies and kinetics, itis dificult for the ration to stay on the target product, ie, ethanol, Because the

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