Sulfur-poisoning on Rh NP but sulfur-promotion on single-Rh1-site for methanol carbonylation

Feng，Siquan1; Mu，Jiali1; Lin，Xiangsong2; Song，Xiangen1; Liu，Siyue1; Shi，Wen1; Zhang，Weiqing3; Wu，Guorong3; Jiayue，Yang3; Dong，Wenrui3; Yang，Xueming3,4; Li，Jingwei1; Jiang，Zheng5; Ding，Yunjie1,6

2023-05-15

10.1016/j.apcatb.2022.122318

APPLIED CATALYSIS B-ENVIRONMENTAL   影响因子和分区

0926-3373

1873-3883

Sulfur poisoning is a severe problem for most noble metal nanoparticle (NP) catalysts, and ppm or ppb levels of sulfur species could result in dramatic activity reduction or even irreversible deactivation. Developing catalysts with high sulfur tolerance is crucial, yet challenging. Here, we reported a clear discovery in methanol carbonylation that sulfur poisoned the Rh NP (Rh/CMK-3) but promoted the single-Rh-site (Rh/AC) while the Rh NP (Rh/AC) experienced a process of atomic dispersion. Strong adsorption of sulfur and the formation of the Rh-S passivation layer were supposed to lead to Rh/CMK-3 sulfur poisoning. However, the detrimental HS transformed into CHSCH and CHSH on Rh/AC and then acted as a ligand of Rh atoms, participating in the subsequent reaction, lowering the energy barrier of the rate-determining step, and lastly promoting the reaction. This work provides benefits in solving the sulfur poisoning of metal NP and developing high sulfur tolerant single-metal-site catalysts.

In situ transformation of H2S Metal nanoparticle catalysts Single-Rh1-site catalyst Sulfur poisoning Sulfur promotion

SCI ; EI

英语

其他

National Natural Science Foundation of China["22002156","22108275","22288201"] ; Youth Innovation Promotion Association of the Chinese Academy of Sciences[2022179] ; CAS Project for Young Scientists in Basic Research[XDB17000000] ; Strategic Priority Research Program of the Chinese Academy of Sciences[121421KYSB20170012] ; International Partnership Program of the Chinese Academy of Sciences[21688102] ; Key Technology Team of the Chinese Academy of Sciences[LY18B060007] ; Natural Science Foundation of Zhejiang Province[GJJSTD20220001] ; Chinese Academy of Sciences[DICP I202237] ; null[YSBR-022]

Chemistry ; Engineering

Chemistry, Physical ; Engineering, Environmental ; Engineering, Chemical

WOS:001001615500001

ELSEVIER

20230213381112

Carbonylation ; Catalyst poisoning ; Methanol ; Nanocatalysts ; Passivation ; Precious metals ; Sulfur

Protection Methods:539.2.1 ; Precious Metals:547.1 ; Nanotechnology:761 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1

CHEMISTRY

2-s2.0-85146081405

Scopus

1.Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
2.School of Materials and Textile Engineering,Jiaxing University,Jiaxing,314001,China
3.State Key Laboratory of Molecular Reaction Dynamics,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China
4.Department of Chemistry,Southern University of Science and Technology,Shenzhen,518055,China
5.Shanghai Synchrotron Radiation Facility,Shanghai Institute of Applied Physics,and Shanghai Advanced Research Institute,Chinese Academy of Sciences,Shanghai,201204,China
6.State Key Laboratory of Catalysis,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian,116023,China

Feng，Siquan,Mu，Jiali,Lin，Xiangsong,et al. Sulfur-poisoning on Rh NP but sulfur-promotion on single-Rh1-site for methanol carbonylation[J]. APPLIED CATALYSIS B-ENVIRONMENTAL,2023,325.

Feng，Siquan.,Mu，Jiali.,Lin，Xiangsong.,Song，Xiangen.,Liu，Siyue.,...&Ding，Yunjie.(2023).Sulfur-poisoning on Rh NP but sulfur-promotion on single-Rh1-site for methanol carbonylation.APPLIED CATALYSIS B-ENVIRONMENTAL,325.

Feng，Siquan,et al."Sulfur-poisoning on Rh NP but sulfur-promotion on single-Rh1-site for methanol carbonylation".APPLIED CATALYSIS B-ENVIRONMENTAL 325(2023).