Citation: Di Xiao-Xia, Zhao Jia, Yu Yi, Xu Xiao-Long, Gu Shan-Chuan, He Hai-Hua, Zhang Tong-Tong, Li Xiao-Nian. One-pot synthesis of nitrogen and sulfur co-doped activated carbon supported AuCl₃ as efficient catalysts for acetylene hydrochlorination[J]. Chinese Chemical Letters, ;2016, 27(9): 1567-1571. doi: 10.1016/j.cclet.2016.03.004 shu

One-pot synthesis of nitrogen and sulfur co-doped activated carbon supported AuCl₃ as efficient catalysts for acetylene hydrochlorination

Institute of Industrial Catalysis of Zhejiang University of Technology, State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology, Hangzhou310032, China

Corresponding author: Li Xiao-Nian, xnli@zjut.edu.cn
Received Date: 14 January 2016
Revised Date: 4 March 2016
Accepted Date: 14 March 2016
Available Online: 14 September 2016

Figures(5)

Commercialization of acetylene hydrochlorination using AuCl₃ catalysts has been impeded by its poor stability. We have been studying that nitrogen-modified Au/NAC catalyst delivered a stable performance which can improve acetylene hydrochlorination activity and has resistance to catalytic deactivation. Here we show that nitrogen and sulfur co-doped activated carbon supported AuCl₃ catalyst worked as efficient catalysts for the hydrochlorination of acetylene to vinyl chloride. Au/NSAC catalyst demonstrated high activity comparative to Au/AC catalyst. Furthermore, it also delivered stable performance within the selectivity of acetylene, reaching more than 99.5%, and there was only a 3.3% C₂H₂ conversion loss after running for 12 h under the reaction conditions of a temperature of 180℃ and a C₂H₂ hourly space velocity of 1480 h 1. The presence of the sulfur atoms may serve to immobilize/anchor the Au and also help prevent reduction and sintering of the Au and hence improve the catalytic activity and stability. The excellent catalytic performance of the Au/NSAC catalyst demonstrated its potential as an alternative to mercury chloride catalysts for acetylene hydrochlorination.
- Acetylene,
- Hydrochlorination,
- AuCl₃,
- Nitrogen and sulfur co-doped
1. [1]
  Hutchings G.J.. Vapor phase hydrochlorination of acetylene:correlation of catalytic activity of supported metal chloride catalysts[J]. J. Catal., 1985,96:292-295. doi: 10.1016/0021-9517(85)90383-5
2. [2]
  Nkosi B., Coville N.J., Hutchings G.J., Nkosi B., Hutchings G.J.. Reactivation of a supported gold catalyst for acetylene hydrochlorination[J]. J. Chem. Soc. Chem. Commun., 1988,1:71-72.
3. [3]
  Nkosi B., Coville N.J., Hutchings G.J.. Vapour phase hydrochlorination of acetylene with group VⅢ and IB metal chloride catalysts[J]. Appl. Catal., 1988,43:33-39. doi: 10.1016/S0166-9834(00)80898-2
4. [4]
  Nkosi B., Adams M.D., Coville N.J., Hutchings G.J.. Hydrochlorination of acetylene using carbon-supported gold catalysts:a study of catalyst reactivation[J]. J. Catal., 1991,128:378-386. doi: 10.1016/0021-9517(91)90296-G
5. [5]
  Nkosi B., Coville N.J., Hutchings G.J.. Hydrochlorination of acetylene using gold catalysts:a study of catalyst deactivation[J]. J. Catal., 1991,128:366-377. doi: 10.1016/0021-9517(91)90295-F
6. [6]
  Conte M., Carley A.F., Heirene C.. Hydrochlorination of acetylene using a supported gold catalyst:a study of the reaction mechanism[J]. J. Catal., 2007,250:231-239. doi: 10.1016/j.jcat.2007.06.018
7. [7]
  Conte M., Carley A.F., Attard G.. Hydrochlorination of acetylene using supported bimetallic Au-based catalysts[J]. J. Catal., 2008,257:190-198. doi: 10.1016/j.jcat.2008.04.024
8. [8]
  Wang S.J., Shen B.X., Song Q.L.. Kinetics of acetylene hydrochlorination over bimetallic Au-Cu/C catalyst[J]. Catal. Lett., 2010,134:102-109. doi: 10.1007/s10562-009-0216-4
9. [9]
  Zhang H.Y., Dai B., Wang X.G., Xu L.L., Zhu M.Y.. Hydrochlorination of acetylene to vinyl chloride monomer over bimetallic Au-La/SAC catalysts[J]. J. Ind. Eng. Chem., 2012,18:49-54. doi: 10.1016/j.jiec.2011.11.075
10. [10]
  Zhang H.Y., Dai B., Wang X.Q.. Non-mercury catalytic acetylene hydrochlorination over bimetallic Au-Co(Ⅲ)/SAC catalysts for vinyl chloride monomer production[J]. Green Chem., 2013,15:829-836. doi: 10.1039/c3gc36840h
11. [11]
  J.Zhao , Xu J.T., Xu J.H.. Activated-carbon-supported gold-cesium(I) ashighly effective catalysts for hydrochlorination of acetylene to vinyl chloride[J]. ChemPlusChem, 2015,80:196-201. doi: 10.1002/cplu.201402176
12. [12]
  Conte M., Davies C.J., Morgan D.J.. Modifications of the metal and support during the deactivation and regeneration of Au/C catalysts for the hydrochlorination of acetylene[J]. Catal. Sci. Technol., 2013,3:128-134. doi: 10.1039/C2CY20478A
13. [13]
  Conte M., Davies C.J., Morgan D.J.. Aqua regia activated Au/C catalysts for the hydrochlorination of acetylene[J]. J. Catal., 2013,297:128-136. doi: 10.1016/j.jcat.2012.10.002
14. [14]
  Zhao J., Xu J.T., Xu J.H.. Enhancement of Au/AC acetylene hydrochlorination catalyst activity and stability via nitrogen-modified activated carbon support[J]. Chem. Eng. J., 2015,262:1152-1160. doi: 10.1016/j.cej.2014.10.071
15. [15]
  Li X.Y., Zhu M.Y., Dai B.. AuCl₃ on polypyrrole-modified carbon nanotubes as acetylene hydrochlorination catalysts[J]. Appl. Catal. B 142-, 2013,143:234-240.
16. [16]
  Johnston P., Carthey N., Hutchings G.J.. Discovery, development, and commercialization of gold catalysts for acetylene hydrochlorination[J]. J. Am. Chem. Soc., 2015,137:14548-14557. doi: 10.1021/jacs.5b07752
17. [17]
  Wang S., Zhang L., Xia Z.. BCN graphene as efficient metal-free electrocatalyst for the oxygen reduction reaction[J]. Angew. Chem. Intern. Ed., 2012,51:4209-4212. doi: 10.1002/anie.201109257
18. [18]
  Liu M.X., Gan L.H., Xiong W.. Partially graphitic micro-and mesoporous carbon microspheres for supercapacitors[J]. Chin. Chem. Lett., 2013,24:1037-1040. doi: 10.1016/j.cclet.2013.07.013
19. [19]
  Cui Z.T., Wang S.G., Zhang Y.H., Cao M.H.. A simple and green pathway toward nitrogen and sulfur dual doped hierarchically porous carbons from ionic liquids for oxygen reduction[J]. J. Power Sources, 2014,259:138-144. doi: 10.1016/j.jpowsour.2014.02.084
20. [20]
  Hakoda T., Yamamoto S., Kawaguchi K.. Oxygen reduction activity of Ndoped carbon-based films prepared by pulsed laser deposition[J]. Appl. Surf. Sci., 2010,257:1556-1561. doi: 10.1016/j.apsusc.2010.08.095
21. [21]
  Deng D.H., Pan X.L., Yu L.. Toward N-doped graphene via solvothermal synthesis[J]. Chem. Mater., 2011,23:1188-1193. doi: 10.1021/cm102666r
22. [22]
  Li X.L., Wang H.L., Robinson J.T.. Simultaneous nitrogen doping and reduction of graphene oxide[J]. J. Am. Chem. Soc., 2009,131:15939-15944. doi: 10.1021/ja907098f
23. [23]
  Wohlgemuth S.A., White R.J., Willinger M.G., Titirici M.M., Antonietti M.. A onepot hydrothermal synthesis of sulfur and nitrogen doped carbon aerogels with enhanced electrocatalytic activity in the oxygen reduction reaction[J]. Green Chem., 2012,14:1515-1523. doi: 10.1039/c2gc35309a
24. [24]
  Su Y.Z., Zhang Y., Zhuang X.D.. Low-temperature synthesis of nitrogen/sulfur co-doped three-dimensional graphene frameworks as efficient metal-free electrocatalyst for oxygen reduction reaction[J]. Carbon, 2013,62:296-301. doi: 10.1016/j.carbon.2013.05.067
25. [25]
  Liu M.X., Deng X.X., Zhu D.Z.. Magnetically separated and N, S co-doped mesoporous carbon microspheres for the removal of mercury ions[J]. Chin. Chem. Lett., 2016,27:795-800. doi: 10.1016/j.cclet.2016.01.038
26. [26]
  Xing L.B., Xi K., Li Q.Y.. Nitrogen, sulfur-codoped graphene sponge as electroactive carbon interlayer for high-energy and -power lithium-sulfur batteries[J]. J. Power Sources, 2016,303:22-28. doi: 10.1016/j.jpowsour.2015.10.097
1. [1]
  Junchen Peng , Xue Yin , Dandan Dong , Zhongyuan Guo , Qinqin Wang , Minmin Liu , Fei He , Bin Dai , Chaofeng Huang . Promotion effect of epoxy group neighboring single-atom Cu site on acetylene hydrochlorination. Chinese Chemical Letters, 2024, 35(6): 109508-. doi: 10.1016/j.cclet.2024.109508
2. [2]
  Yongsheng Xu , Lisha Yao , Jian Li , Yanzhao Dong , Dongyang Xie , Miaomiao Zhang , Feng Li , Yunsheng Dai , Jinli Zhang , Haiyang Zhang . Dual-ligand engineering over Au-based catalyst for efficient acetylene hydrochlorination. Chinese Chemical Letters, 2025, 36(3): 110318-. doi: 10.1016/j.cclet.2024.110318
3. [3]
  Yusheng Lu , Chaofeng Huang , Zhigang Lei , Mingyuan Zhu . Catalytic effects of structural design in N-modified carbon materials for the hydrochlorination of acetylene. Chinese Chemical Letters, 2025, 36(8): 110583-. doi: 10.1016/j.cclet.2024.110583
4. [4]
  Junchen Peng , Zhongyuan Guo , Dandan Dong , Yusheng Lu , Bao Wang , Fangjie Lu , Chaofeng Huang , Bin Dai . Cu⁰/Cu^δ⁺ site construction and its catalytic role in acetylene hydrochlorination. Chinese Chemical Letters, 2025, 36(8): 111208-. doi: 10.1016/j.cclet.2025.111208
5. [5]
  Linfeng Li , Bao Wang , Tiantong Zhang , Xinyuan Wang , Dingqiang Feng , Wei Li , Jiangjiexing Wu , Jinli Zhang . Identifying the catalytic active site of durable Ru-based liquid-phase catalyst for acetylene hydrochlorination. Chinese Chemical Letters, 2025, 36(10): 111303-. doi: 10.1016/j.cclet.2025.111303
6. [6]
  Yanhui Lu , Chengang Pei , Wenqiang Li , Qing Liu , Huan Pang , Xu Yu . Tailoring active sites of cerium and nitrogen Co-doped rhenium disulfide for enhanced hydrogen evolution reaction. Chinese Chemical Letters, 2025, 36(12): 111646-. doi: 10.1016/j.cclet.2025.111646
7. [7]
  Jiaojiao Liang , Youming Peng , Zhichao Xu , Yufei Wang , Menglong Liu , Xin Liu , Di Huang , Yuehua Wei , Zengxi Wei . Boron/phosphorus co-doped nitrogen-rich carbon nanofiber with flexible anode for robust sodium-ion battery. Chinese Chemical Letters, 2025, 36(1): 110452-. doi: 10.1016/j.cclet.2024.110452
8. [8]
  Huiying LIN , Xiang ZHAO , Banghao WEI , Bufeng WANG , Zhiyong LU , Junfeng BAI . Perfluroalkane functionalization on MOF-808 for acetylene purification. Chinese Journal of Inorganic Chemistry, 2025, 41(10): 2103-2114. doi: 10.11862/CJIC.20250110
9. [9]
  Jie XIE , Hongnan XU , Jianfeng LIAO , Ruoyu CHEN , Lin SUN , Zhong JIN . Nitrogen-doped 3D graphene-carbon nanotube network for efficient lithium storage. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 1840-1849. doi: 10.11862/CJIC.20240216
10. [10]
  Xiping Dong , Xuan Wang , Zhixiu Lu , Qinhao Shi , Zhengyi Yang , Xuan Yu , Wuliang Feng , Xingli Zou , Yang Liu , Yufeng Zhao . Construction of Cu-Zn Co-doped layered materials for sodium-ion batteries with high cycle stability. Chinese Chemical Letters, 2024, 35(5): 108605-. doi: 10.1016/j.cclet.2023.108605
11. [11]
  Junmei FAN , Wei LIU , Ruitao ZHU , Chenxi QIN , Xiaoling LEI , Haotian WANG , Jiao WANG , Hongfei HAN . High sensitivity detection of baicalein by N, S co-doped carbon dots and their application in biofluids. Chinese Journal of Inorganic Chemistry, 2024, 40(10): 2009-2020. doi: 10.11862/CJIC.20240120
12. [12]
  Hangwen Zheng , Ziqian Wang , HuiJie Zhang , Jing Lei , Rihui Li , Jian Yang , Haiyan Wang . Synthesis and applications of B, N co-doped carbons for zinc-based energy storage devices. Chinese Chemical Letters, 2025, 36(3): 110245-. doi: 10.1016/j.cclet.2024.110245
13. [13]
  Xuehua SUN , Min MA , Jianting LIU , Rui TIAN , Hongmei CHAI , Huali CUI , Loujun GAO . Pr/N co-doped biomass carbon dots with enhanced fluorescence for efficient detection of 2,4-dinitrophenylhydrazine. Chinese Journal of Inorganic Chemistry, 2025, 41(3): 561-573. doi: 10.11862/CJIC.20240294
14. [14]
  Chunxiu Yu , Zelin Wu , Hongle Shi , Lingyun Gu , Kexin Chen , Chuan-Shu He , Yang Liu , Heng Zhang , Peng Zhou , Zhaokun Xiong , Bo Lai . Insights into the electron transfer mechanisms of peroxydisulfate activation by modified metal-free acetylene black for degradation of sulfisoxazole. Chinese Chemical Letters, 2024, 35(8): 109334-. doi: 10.1016/j.cclet.2023.109334
15. [15]
  Shaoming Dong , Yiming Niu , Yinghui Pu , Yongzhao Wang , Bingsen Zhang . Subsurface carbon modification of Ni-Ga for improved selectivity in acetylene hydrogenation reaction. Chinese Chemical Letters, 2024, 35(12): 109525-. doi: 10.1016/j.cclet.2024.109525
16. [16]
  Yining Li , Shimei Wu , Lantao Chen , Haosen Fan , Yufei Zhang , Lingxing Zeng . Multiple yolks-shell cobalt phosphosulfide nanocrystals encapsulating into rich heteroatoms co-doped carbon frameworks for advanced sodium/potassium ion batteries. Chinese Chemical Letters, 2025, 36(9): 110371-. doi: 10.1016/j.cclet.2024.110371
17. [17]
  Menglin Zhou , Lin Zhang , Xuefei Shan , Fengqin Chang , Wentong Chen , Xuguang An , Guangzhi Hu . Hydrangea-like B/N co-doped carbon-based electrochemical sensors for the efficient and sensitive detection of aristolochic acid in Aristolochia. Chinese Chemical Letters, 2025, 36(12): 111073-. doi: 10.1016/j.cclet.2025.111073
18. [18]
  Hongzhe GUO , Sen WANG , Lu YANG , Fucheng LIU , Jiongpeng ZHAO , Zhaoquan YAO . Highly selective acetylene capture by a pacs-type metal-organic framework constructed using metal-formate complexes as pore partition units. Chinese Journal of Inorganic Chemistry, 2025, 41(10): 2157-2164. doi: 10.11862/CJIC.20250179
19. [19]
  Tian TIAN , Meng ZHOU , Jiale WEI , Yize LIU , Yifan MO , Yuhan YE , Wenzhi JIA , Bin HE . Ru-doped Co₃O₄/reduced graphene oxide: Preparation and electrocatalytic oxygen evolution property. Chinese Journal of Inorganic Chemistry, 2025, 41(2): 385-394. doi: 10.11862/CJIC.20240298
20. [20]
  Yifen He , Chao Qu , Na Ren , Dawei Liang . Enhanced degradation of refractory organics in ORR-EO system with a blue TiO₂ nanotube array modified Ti-based Ni-Sb co-doped SnO₂ anode. Chinese Chemical Letters, 2024, 35(8): 109262-. doi: 10.1016/j.cclet.2023.109262

Get Citation

PDF

XML

Metrics

PDF Downloads(1)
Abstract views(1085)
HTML views(18)

通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

One-pot synthesis of nitrogen and sulfur co-doped activated carbon supported AuCl3 as efficient catalysts for acetylene hydrochlorination

Metrics

通讯作者: 陈斌, bchen63@163.com

One-pot synthesis of nitrogen and sulfur co-doped activated carbon supported AuCl₃ as efficient catalysts for acetylene hydrochlorination