单原子催化: 追寻催化领域的“圣杯”

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

催化学报 ›› 2023, Vol. 52: 1-13.DOI: 10.1016/S1872-2067(23)64505-X

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单原子催化: 追寻催化领域的“圣杯”

王思恺^a^,^b^,¹, 闵祥婷^c^,¹, 乔波涛^c^,^d, 颜宁^a^,^b^,^*(), 张涛^c^,^d^,^e^,^*()

^a天津大学滨海新城国际校区, 新加坡国立大学与天津大学联合学院, 福建福州350207, 中国
^b新加坡国立大学化学与生物分子工程系, 新加坡
^c中国科学院大连化学物理研究所, 中国科学院应用催化科学技术重点实验室, 辽宁大连116023, 中国
^d中国科学院大学, 北京100049, 中国
^e中国科学院大连化学物理研究所, 催化基础国家重点实验室, 辽宁大连116023, 中国

收稿日期:2023-07-14 接受日期:2023-08-21 出版日期:2023-09-18 发布日期:2023-09-25
通讯作者: *电子信箱: ning.yan@nus.edu.sg (颜宁),taozhang@dicp.ac.cn (张涛).
作者简介:¹共同第一作者.

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.

摘要/Abstract

摘要：

在催化领域, “圣杯”反应是指对人类未来具有显著的科学、经济和环境可持续性价值的反应. 这些反应利用地球上丰富易得的资源, 如CH₄, H₂O, CO₂和N₂等, 生产各种有价值的化工产品. 尽管意义重大, 但由于反应物的化学惰性和产物相对活泼的特点, 反应的转化率通常较低, 对目标产物的选择性较差. 目前, 降低“圣杯”反应的活化能垒仍然是一个巨大的挑战, 需要开发新型催化剂来应对以上挑战. 单原子催化剂(SAC)含有部分带电的金属单原子物种, 具有明确的、可调的结构, 是一类很有前途的负载型催化剂, 不仅可以提升催化性能, 也为深入了解反应机制和构效关系提供便利.

本文总结和评价了SAC在五个“圣杯”反应中的最新应用. 围绕甲烷活化, 介绍了甲烷温和氧化制甲醇和无氧甲烷偶联两类反应. 热催化甲烷氧化通常需要引入共还原剂来提升催化活性, 因此所采用的SAC通过多位点协同作用, 实现串联催化过程以有效活化甲烷; 而光催化过程则可在无共还原剂的情况下, 通过不同单原子金属位点(如Au, Pd, Fe, W)与水或O₂的作用, 产生活性氧物种, 实现甲烷活化. 目前用于甲烷氧化的SAC仍缺乏统一的设计和优化标准, 在效率提升和机理研究等方面有很大发展空间. 对于无氧甲烷偶联反应, 目前开发的SAC主要有Fe, Pt和Pd基催化剂, 其中单原子位点有助于抑制积碳, 提升性能稳定性和产物选择性. 然而, 部分SAC在高温无氧气氛下难以维持其单原子结构, 仍需进一步探索和优化. 随后介绍了两种人工光合成反应, 即水分解产氢和CO₂还原. 对于光催化产氢, SAC独特且结构明确的位点可显著提升产氢乃至全解水的性能, 也可用于产氢机理的深入研究. 对于光催化CO₂还原, 重点介绍了对生成CO, CH₄和CH₃OH具有高选择性的SAC, 其中, 单原子位点对于调节小分子中间体的吸附起到了重要作用, 从而影响了选择性. 许多用于人工光合成的SAC存在不止一种催化位点, 这些位点可以协同提升目标反应的效率. 最后, 展示了SAC用于氮气活化合成氨的研究进展, 大多采用非贵金属位点(如Fe, Co和La), 通过特定的配位结构实现与N₂的特殊作用, 以有效削弱N≡N键强度.

本文最后总结了SAC在“圣杯”反应中的优势和面临的诸多挑战, 并提出了该领域未来可能的发展方向, 其中包括深入探究机理和构效关系, 结合先进信息技术高效筛选符合条件的催化剂, 以及设计新型催化位点以扩大催化材料的应用领域.

关键词: 单原子催化剂, 人工光合成, 选择性甲烷氧化, 无氧甲烷偶联, 光催化制氢, 二氧化碳光还原, 氮气活化

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

王思恺, 闵祥婷, 乔波涛, 颜宁, 张涛. 单原子催化: 追寻催化领域的“圣杯”[J]. 催化学报, 2023, 52: 1-13.

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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图/表 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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单原子催化: 追寻催化领域的“圣杯”

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

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