Structure Sensitivity of CO2 Hydrogenation on Ni Revisited DOI Creative Commons

Jérôme F. M. Simons,

Ton J. de Heer,

Rim C. J. van de Poll

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(37), С. 20289 - 20301

Опубликована: Сен. 7, 2023

Despite the large number of studies on catalytic hydrogenation CO2 to CO and hydrocarbons by metal nanoparticles, nature active sites reaction mechanism have remained unresolved. This hampers development effective catalysts relevant energy storage. By investigating structure sensitivity a set silica-supported Ni nanoparticle (2-12 nm), we found that responsible for conversion are different from those subsequent CH4. While former step is weakly dependent size, latter strongly sensitive with particles below 5 nm losing their methanation activity. Operando X-ray diffraction absorption spectroscopy results showed significant oxidation or restructuring, which could be observed differences in rates, was absent. Instead, decreased activity related higher selectivity small nanoparticles linked lower availability edges dissociation. infrared coupled (isotopic) transient experiments revealed dynamics surface species during demonstrated direct dissociation followed bonded carbonyls These findings provide essential insights into much debated reactions key knowledge-driven design highly selective catalysts.

Язык: Английский

Advancement of modification engineering in lean methane combustion catalysts based on defect chemistry DOI
Ruishan Qiu, Wei Wang, Zhe Wang

и другие.

Catalysis Science & Technology, Год журнала: 2023, Номер 13(8), С. 2566 - 2584

Опубликована: Янв. 1, 2023

This review takes defect chemistry as the starting point and improvement of material properties foothold, puts forward insights on application, limitation prospect engineering in modification methane combustion catalysts.

Язык: Английский

Процитировано

53
Gas-Dependent Active Sites on Cu/ZnO Clusters for CH3OH Synthesis DOI
Weifeng Tu,

Pengchao Ren,

Yuanjie Li

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(16), С. 8751 - 8756

Опубликована: Март 21, 2023

This study describes an instantaneously gas-induced dynamic transition of industrial Cu/ZnO/Al2O3 catalyst. Cu/ZnO clusters become "alive" and lead to a promotion in reaction rate by almost one magnitude, response the variation reactant components. The promotional changes are functions either CO2-to-CO or H2O-to-H2 ratio which determines oxygen chemical potential thus drives undergo reconstruction allows maximum formation Cu-Zn2+ sites for CH3OH synthesis.

Язык: Английский

Процитировано

53
Machine-learning atomic simulation for heterogeneous catalysis DOI Creative Commons
Dongxiao Chen, Cheng Shang, Zhi‐Pan Liu

и другие.

npj Computational Materials, Год журнала: 2023, Номер 9(1)

Опубликована: Янв. 7, 2023

Abstract Heterogeneous catalysis is at the heart of chemistry. New theoretical methods based on machine learning (ML) techniques that emerged in recent years provide a new avenue to disclose structures and reaction complex catalytic systems. Here we review briefly history atomic simulations then focus trend shifting toward ML potential calculations. The advanced developed by our group are outlined illustrate how networks can be resolved using combination with efficient global optimization methods. future simulation outlooked.

Язык: Английский

Процитировано

52
Influencing electrocatalytic processes through topographically disordered atomic sites DOI Creative Commons

P. Prabhu,

Jong‐Min Lee

Chem Catalysis, Год журнала: 2023, Номер 3(6), С. 100621 - 100621

Опубликована: Май 11, 2023

Язык: Английский

Процитировано

49
Structure Sensitivity of CO2 Hydrogenation on Ni Revisited DOI Creative Commons

Jérôme F. M. Simons,

Ton J. de Heer,

Rim C. J. van de Poll

и другие.

Journal of the American Chemical Society, Год журнала: 2023, Номер 145(37), С. 20289 - 20301

Опубликована: Сен. 7, 2023

Despite the large number of studies on catalytic hydrogenation CO2 to CO and hydrocarbons by metal nanoparticles, nature active sites reaction mechanism have remained unresolved. This hampers development effective catalysts relevant energy storage. By investigating structure sensitivity a set silica-supported Ni nanoparticle (2-12 nm), we found that responsible for conversion are different from those subsequent CH4. While former step is weakly dependent size, latter strongly sensitive with particles below 5 nm losing their methanation activity. Operando X-ray diffraction absorption spectroscopy results showed significant oxidation or restructuring, which could be observed differences in rates, was absent. Instead, decreased activity related higher selectivity small nanoparticles linked lower availability edges dissociation. infrared coupled (isotopic) transient experiments revealed dynamics surface species during demonstrated direct dissociation followed bonded carbonyls These findings provide essential insights into much debated reactions key knowledge-driven design highly selective catalysts.

Язык: Английский

Процитировано

49