Single-atom catalysts: In search of the holy grails in catalysis

doi:10.1016/S1872-2067(23)64505-X

Chinese Journal of Catalysis ›› 2023, Vol. 52: 1-13.DOI: 10.1016/S1872-2067(23)64505-X

• Perspective • Next Articles

Single-atom catalysts: In search of the holy grails in catalysis

Sikai Wang^a^,^b^,¹, Xiang-Ting Min^c^,¹, Botao Qiao^c^,^d, Ning Yan^a^,^b^,^*(), Tao Zhang^c^,^d^,^e^,^*()

^aJoint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Binhai New City, Fuzhou 350207, Fujian, China
^bDepartment of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive, Singapore
^cCAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^dUniversity of Chinese Academy of Sciences, Beijing 100049, China
^eState Key Laboratory of Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China

Received:2023-07-14 Accepted:2023-08-21 Online:2023-09-18 Published:2023-09-25
Contact: *E-mail: ning.yan@nus.edu.sg (N. Yan),taozhang@dicp.ac.cn (T. Zhang).
About author:Ning Yan (Department of Chemical & Biomolecular Engineering, National University of Singapore) currently holds a Dean’s Chair Professorship at National University of Singapore. He received his B.Sc. and Ph.D. degrees in chemistry from Peking University (China) in 2004 and 2009, respectively (supervisor: Prof. Yuan Kou). Then he joined the École Polytechnique Fédérale de Lausanne in Switzerland with a Marie Curie Fellowship until 2012 (collaborator: Prof. Paul Dyson). After that, he started working in the Department of Chemical and Biomolecular Engineering in National University of Singapore and was promoted to a tenured associate professor in 2018. He received NRF Investigatorship Award (2022), NUS Young Researcher Award (2019), ACS Sustainable Chemistry & Engineering Lectureship Award (2018), and RSC Environment, Sustainability and Energy Early Career Award (2017), among others. His research interests lie in advanced heterogeneous catalysis, green chemistry & engineering, and renewable energy & chemical production, with over 200 published peer-reviewed papers.
Tao Zhang (Dalian Institute of Chemical Physics, Chinese Academy of Sciences) received his Ph.D. in physical chemistry from Dalian Institute of Chemical Physics (DICP) in 1989 under the supervision of Prof. Liwu Lin. After a one-year postdoctoral position with Prof. Frank Berry at Birmingham University, he founded his own group at DICP in 1990 and promoted to full professor there in 1995. Prof. Zhang was the director of DICP in 2007-2017 and has been a vice president of Chinese Academy of Sciences since 2017. He was appointed as the editors-in-chief of Chin. J. Catal. in 2014. Meanwhile, he has been the director representing the China aside of the China-France Joint laboratory for Sustainable Energy since 2008. Prof. Zhang has won many important awards, such as the National Invention Prize (for three times), Distinguished Award of CAS, Excellent Scientist Award of Chinese Catalysis Society, and Ho Leung Ho Lee Prize for Science and Technology. His research interests focus on heterogeneous catalysis, environmental catalysis, and biomass conversion. He authored and coauthored more than 400 publications in peer-reviewed journals.
¹Contribute equally to this work.

Abstract

Abstract:

This perspective assesses the recent progress using single-atom catalysts for five “holy grail” reactions, including partial methane oxidation to methanol, non-oxidative methane conversion, photocatalytic CO₂ reduction, photocatalytic water splitting, and nitrogen activation. Using selected case studies, we discuss promising efforts in these domains and at the same time identify the remaining challenges in using SACs for selective and efficient chemical transformations across thermal, electrical, and light-driven catalysis. Looking forward, we highlight the significant potential of SAC research in areas like mechanistic studies, high-throughput screening, and novel catalytic system design.

Key words: Single-atom catalyst, Artificial photosynthesis, Selective methane oxidation, Non-oxidative methane coupling, Photocatalytic hydrogen production, Carbon dioxide photoreduction, Nitrogen activation

Sikai Wang, Xiang-Ting Min, Botao Qiao, Ning Yan, Tao Zhang. Single-atom catalysts: In search of the holy grails in catalysis[J]. Chinese Journal of Catalysis, 2023, 52: 1-13.

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Figures/Tables 4

Fig. 1. Statistics of published articles about adopting SACs for direct conversion of methane, water, carbon dioxide and nitrogen into value-added chemicals via thermo-catalysis, electrocatalysis or photo(electro)catalysis (using Scopus database, data collected on 30th June 2023).

Fig. 2. Single atom catalysts for direct methane conversion. (a) Scheme of proposed reaction pathway for partial oxidation of CH4 with O2 and H2 over PdCu/Z-5. Reprinted with permission from Ref. [31]. Copyright 2022, John Wiley and Sons. (b) Reaction pathway for partial oxidation of methane over Au1/BP nanosheets under light irradiation. The inset images show the side views of the configurations. Yellow, violet, pink, red, gray, and white spheres refer to Au, surface P, subsurface P, O, C, and H atoms, respectively. Reprinted with permission from Ref. [37]. Copyright 2021, Springer Nature. (c) Schematic showing selective photo-activation of CH4 to CH3OH over PMOF-RuFe(OH) in the presence of O2, H2O and irradiation (hν). (d) Comparison of the methane oxidation activity over various catalysts in batch mode. Reaction conditions: 3 mL water, 20 h visible light, 10 mg catalyst and CH4/O2 (1 atm). Figs. (c) and (d) are reprinted with permission from Ref. [39]. Copyright 2022, Springer Nature. (e) Free-energy profiles of intermediates and transition states for methane activation and transformation on Fe1?SiC2 active center. Reprinted with permission from Ref. [51]. Copyright 2020, John Wiley and Sons. (f) Comparison of nonoxidative methane conversion activity and product selectivity at 975 °C over the different catalysts and controls. Reprinted with permission from Ref. [52]. Copyright 2018, American Chemical Society. (g) Time-dependent photocatalytic C2H6 and C2H4 production over ZnO-AuPd2.7%. Reprinted with permission from Ref. [60]. Copyright 2021, American Chemical Society.

Fig. 3. Selected SACs systems very recently for artificial photosynthesis. (a) H2 evolution rates of the CN@CuS, Pt@CN@CuS and Pt1-CN@CuS. Reprinted with permission from Ref. [77]. Copyright 2020, John Wiley and Sons. (b) UV/Vis-NIR DRS spectra of prepared samples. (c) H2 evolution tests of prepared samples under visible light irradiation (λ > 430 nm) at 30 °C. Figs. (b) and (c) are reprinted with permission from Ref. [81]. Copyright 2022, John Wiley and Sons. (d) Mass distributions of C60V+, C60VO+, and C60V+(H2O) produced via laser vaporization, with and without IR irradiation at 1190 cm-1. (e) IRMPD spectrum of C60V+(H2O) and calculated spectra of C60V+(H2O) with η5 and η6. Figs. (d) and (e) are reprinted with permission from Ref. [82]. Copyright 2021, John Wiley and Sons. (f) Photocatalytic CO evolution over different Fe catalyst. Reprinted with permission from Ref. [88]. Copyright 2022, American Chemical Society. (g) Gas yield and selectivity towards methane for PCN‐Cu SACs, PCN‐Ru SACs and PCN‐RuCu SACs. (h) Schematic of the possible photocatalytic mechanism of PCN‐RuCu for photocatalytic CO2 reduction under light illumination. Nitrogen, carbon, ruthenium and copper atoms are shown in blue, gray, green and pale red, respectively. Figs. (g) and (h) are reprinted with permission from Ref. [90]. Copyright 2022, Elsevier B. V. (i) Production rates of CH4 and CO of CO2 photoreduction for Pd1/C3N4, Pd1+NPs/C3N4, and PdNPs/C3N4. (j) The reaction mechanism for photoreduction of CO2 to CH4 over Pd1+NPs/C3N4. Figs. (i) and (j) are reprinted with permission from Ref. [91]. Copyright 2022, John Wiley and Sons.

Fig. 4. N2 hydrogenation pathway on the steady-state Co1-N3.5 sites (represented by A) (a) and dynamic cyclic sites (CoN6?x/C) (b). Figs. (a) and (b) are reprinted with permission from Ref. [100]. Copyright 2020, Springer Nature. (c) Molecular orbital diagram of N2 and proposed Fe spin configurations in FeN4 and FeN3S1. Reprinted with permission from Ref. [104]. Copyright 2022, John Wiley and Sons. (d) DFT-calculated optimized free energy pathways for NRR on FeS2O2, FeS1O3, FeS1O2 and FeO3 coordination configurations, respectively. Reprinted with permission from Ref. [105]. Copyright 2022, John Wiley and Sons. (e) Diagrams of the nitrogen π* 2p orbital and the electron transfer from La to the adsorbed nitrogen. Reprinted with permission from Ref. [109]. Copyright 2022, Elsevier B. V.

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Single-atom catalysts: In search of the holy grails in catalysis

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