CO₂-Assisted Dehydrogenation of Propane by Atomically Dispersed Pt on MXenes

Chu, Changqing1; Chen, Baoyu1; He, Yan1,2; Jiang, Guiyuan3; Lan, Xingying3; Li, Shenggang4,5; Wu, Changning6,7; Cao, Daofan8

2024-06-12

10.1021/acscatal.4c01473

ACS CATALYSIS   影响因子和分区

2155-5435

The catalytic mechanism and performance of MXene-supported atomically dispersed Pt (Pt-1@MXene) in CO2-assisted propane oxidative dehydrogenation (CO2-ODHP) was evaluated by density functional theory (DFT) calculations and microkinetic simulations. The Pt single atom (Pt SA) site can promote the cleavage of two C-H bonds in propane to yield propylene via direct dehydrogenation of propane (DDHP), whereas the Pt-MXene interface facilitates the cleavage of the C-O bond in CO2 and the hydrogenation of O* to H2O via the reverse water gas shift (RWGS). Degree of rate control and Br & ouml;nsted-Evans-Polanyi (BEP) correlation analyses revealed that the binding strength of Pt toward C3H7* and that of MXene toward O* determined the DDHP and RWGS activities, respectively. The DDHP activity is also highly correlated with the d-band center of the Pt SA and the work function of the Pt-1@MXene surface. Microkinetic simulations showed that the Pt SA anchored on Mo2CO2 and W2CO2 possessed superior DDHP activity than the Pt(111) surface, although only Pt-1@Mo2CO2 presented high activities in both DDHP and RWGS. Furthermore, the high energy barriers of deep dehydrogenations and C-C cracking of C-3 derivatives over Pt-1@Mo2CO2 evidenced its high anticoking ability. These predictions suggest Pt-1@Mo2CO2 as a promising CO2-ODHP catalyst.

CO2-assisted propane dehydrogenation catalystdesign MXene single atom catalysts DFTcalculations microkinetic simulations

SCI ; EI

英语

其他

National Natural Science Foundation of China["52336003","U22B20149","22172188","22293023","22293025"] ; National Natural Science Foundation of China[WX20230151] ; Special Expert Project of Shandong Province Taishan Scholars Program["23YF1453400","23ZR1481700"]

Chemistry

Chemistry, Physical

WOS:001247387800001

AMER CHEMICAL SOC

20242516278090

Catalysts ; Chemical shift ; Dehydrogenation ; Density functional theory ; Design for testability ; Platinum ; Propane ; Water gas shift

Precious Metals:547.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.Qingdao Univ Sci & Technol, Coll Electromech Engn, Qingdao 266061, Peoples R China
2.Qingdao Univ, Qingdao 266061, Peoples R China
3.China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
4.Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
5.Chinese Acad Sci, Shanghai Adv Res Inst, State Key Lab Low Carbon Catalysis & Carbon Dioxid, Shanghai 201210, Peoples R China
6.Southern Univ Sci & Technol, Coll Innovat & Entrepreneurship, Shenzhen 518055, Peoples R China
7.Beijing Petrochem Engn Co Ltd BPE, Beijing 100107, Peoples R China
8.Univ Birmingham, Birmingham Ctr Energy Storage BCES, Birmingham B15 2TT, England

Chu, Changqing,Chen, Baoyu,He, Yan,et al. CO₂-Assisted Dehydrogenation of Propane by Atomically Dispersed Pt on MXenes[J]. ACS CATALYSIS,2024,14(13):9662-9677.

Chu, Changqing.,Chen, Baoyu.,He, Yan.,Jiang, Guiyuan.,Lan, Xingying.,...&Cao, Daofan.(2024).CO₂-Assisted Dehydrogenation of Propane by Atomically Dispersed Pt on MXenes.ACS CATALYSIS,14(13),9662-9677.

Chu, Changqing,et al."CO₂-Assisted Dehydrogenation of Propane by Atomically Dispersed Pt on MXenes".ACS CATALYSIS 14.13(2024):9662-9677.