用于电化学能量转换反应的非贵金属单原子催化剂

doi:10.1016/S1872-2067(23)64456-0

催化学报 ›› 2023, Vol. 50: 195-214.DOI: 10.1016/S1872-2067(23)64456-0

用于电化学能量转换反应的非贵金属单原子催化剂

Sang Eon Jun^a^,^b, Sungkyun Choi^a, Jaehyun Kim^a, Ki Chang Kwon^b^,^*(), Sun Hwa Park^b^,^*(), Ho Won Jang^a^,^c^,^*()

^a首尔国立大学先进材料研究所, 材料科学与工程系, 首尔, 韩国
^b韩国标准与科学研究院跨学科材料测量研究所, 大田, 韩国
^c首尔国立大学融合技术高级研究所, 水原, 韩国

收稿日期:2023-03-15 接受日期:2023-05-15 出版日期:2023-07-18 发布日期:2023-07-25
通讯作者: *电子信箱: kichang.kwon@kriss.re.kr (K. C. Kwon), PSH@kriss.re.kr (S. H. Park), hwjang@snu.ac.kr (H. W. Jang).

Non-noble metal single atom catalysts for electrochemical energy conversion reactions

Sang Eon Jun^a^,^b, Sungkyun Choi^a, Jaehyun Kim^a, Ki Chang Kwon^b^,^*(), Sun Hwa Park^b^,^*(), Ho Won Jang^a^,^c^,^*()

^aDepartment of Materials Science and Engineering, Research Institute of Advanced Materials, Seoul National University, Seoul 08826, Republic of Korea
^bInterdisciplinary Materials Measurement Institute, Korea Research Institute of Standards and Science, Daejeon 34113, Republic of Korea
^cAdvanced Institute of Convergence Technology, Seoul National University, Suwon 16229, Republic of Korea

Received:2023-03-15 Accepted:2023-05-15 Online:2023-07-18 Published:2023-07-25
Contact: *E-mail: kichang.kwon@kriss.re.kr (K. C. Kwon), PSH@kriss.re.kr (S. H. Park),hwjang@snu.ac.kr (H. W. Jang).
About author:Ki Chang Kwon is a Senior Research Scientist of the Interdisciplinary Materials Measurement Institute in Korea Research Institute of Standards and Science (KRISS). He earned his Ph.D. from the Department of Materials Science and Engineering in Seoul National University in 2018 under supervision of prof. Ho Won Jang. He worked as a Postdoctoral research staff at Seoul National University at 2018 and at National University of Singapore (NUS) from 2018 to 2021. His research interests include the synthesis of low dimensional materials (1D & 2D), and halide perovskites, and their applications for nanoelectronics, solar water splitting catalysts, and chemoresistive gas sensors.
Sun Hwa Park (Korea Research Institute of Standards and Science) received her Ph.D from the Nanomaterials Science and Engineering at University of Science and Technology in 2013. She joined Korea Research Institute of Standards and Science as a senior research scientist in 2014 and became a principal research scientist in 2023. She worked at the University of California at Riverside as a visiting scholar in 2018. Her research interests currently focus on the synthesis of nanoengineered materials based on electrochemistry and the application of these materials in a variety of fields including electrocatalysis, energy storage systems and sensors. Her recent ongoing research includes the development of reliable electrochemical measurement and evaluation techniques related to water electrolysis system and lithium-ion batteries.
Ho Won Jang is a full professor in Department of Materials Science and Engineering at Seoul National University. He earned his Ph.D from the Department of Materials Science and Engineering of Pohang University of Science and Technology in 2004. He worked as a research associate at University of Madison-Wisconsin from 2006 to 2009. Before he joined Seoul National University in 2012, he had worked at Korea Institute of Science and Technology as a senior research scientist. He is a member of Young Korean Academy of Science and Technology and is serving as an associate editor for journals, Exploration and Eco Energy. His research interests include materials synthesis and device fabrication for solar fuel generation, chemical sensing, nonvolatile data storage, neuromorphic computing, plasmonics, ferroelectronics, and metal-insulator transition. He has published more than 500 papers in international refereed journals.

摘要/Abstract

摘要：

非贵金属单原子催化剂(NNMSAC)被认为是贵金属单原子催化剂的经济替代品, 同时保留了源自单原子位点独特电子结构的高催化活性. 通过金属-载体充分的相互作用, NNMSAC可以在各种电催化反应中发挥关键作用, 具有与贵金属单原子催化剂相当的高原子利用效率和选择性. 为此, 本文首先综述了NNMSAC在调节反应选择性、金属-载体相互作用和催化活性中心方面的特点. 随后, 详细介绍了用于析氢反应、析氧反应、氧还原反应、二氧化碳还原反应和氮还原反应的代表性NNMSAC(Co, Ni, Fe, Cu和双金属SAC)催化剂. 最后, 展望了NNMSAC在几何、电子和电化学性能方面进一步发展所面临的挑战.

关键词: 单原子催化剂, 非贵金属, 电催化, 水裂解, CO₂还原

Abstract:

Non-noble metal single atom catalysts (NNMSACs) are being pursued as economical alternatives to noble-metal SACs while retaining the high catalytic activity derived from the unique electronic structure of the single atomic sites. NNMSACs can serve crucial roles in various electrocatalytic reactions with high atomic utilization efficiency and selectivity comparable to noble metal SACs via adequate metal-support interactions. To this end, this review summarizes the characteristics of NNMSACs with regard to tuning reaction selectivity, metal-support interaction, and catalytic active center. Subsequently, an extensive summary of representative NNMSACs (Co, Ni, Fe, Cu, and dual metal SACs) is introduced for hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO₂RR), and nitrogen reduction reaction (NRR). Finally, we present a brief conclusion and the remaining challenges for further advances of NNMSACs in geometric, electronic, and electrochemical properties.

Key words: ingle atom catalysts, Non-noble metals, Electrocatalysis, Water splitting, CO₂ reduction

Sang Eon Jun, Sungkyun Choi, Jaehyun Kim, Ki Chang Kwon, Sun Hwa Park, Ho Won Jang. 用于电化学能量转换反应的非贵金属单原子催化剂[J]. 催化学报, 2023, 50: 195-214.

Sang Eon Jun, Sungkyun Choi, Jaehyun Kim, Ki Chang Kwon, Sun Hwa Park, Ho Won Jang. Non-noble metal single atom catalysts for electrochemical energy conversion reactions[J]. Chinese Journal of Catalysis, 2023, 50: 195-214.

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图/表 13

Fig. 1. A schematic of the ultimate target for non-noble-metal SACs with excellent catalytic performance.

Fig. 2. A schematic of earth-abundant transition metal elements in periodic table utilized for single atom catalysts in electrocatalysis.

Fig. 3. (a) HAADF-STEM image of Co-C3N4/rGO. (b) XANES spectra at the Co K-edge of Co foil, CoO, Co3O4, CoPc, and Co-C3N4/rGO. (c) FT-EXAFS spectra in R space. (d) LSV curves of Co-C3N4/rGO, Co-C3N4, C3N4/rGO, and Pt/C in 1.0 mol L?1 KOH. (e) Mass activity of Co-C3N4, Pt-C, and Co-C3N4/rGO at the overpotential of 30, 40, 50, and 60 mV. (f) Free energy diagrams of OER on Co-3N and Co-N model. Reprinted with permission from Ref. [50]. Copyright 2022, American Chemical Society.

Fig. 4. (a) HAADF-STEM image of CN-0.5 Ni-HO. (b) FT-EXAFS spectra at the Ni K-edge of Ni foil, NiO, and Ni single atom coordinated CN with various Ni contents from 0.1% to 0.5%. (c) XANES spectra at the Ni K-edge. (d) Density of states of CN and CN-0.2Ni-HO. (e) Work functions of CN and CN-0.2Ni-HO. (f) Photocatalytic H2 production rates of CN, CN-Ni particles, and CN-0.2Ni-HO. Reprinted with permission from Ref. [51]. Copyright 2020, Wiley-VCH.

Fig. 5. (a) Synthesis schematic of Ni-O-G SACs. (b) FT-EXAFS spectra of Ni-O-G SACs with references of NiO and Ni foil. (c) The OER current curves of Ni-O-G SACs, NiO, B Ni-O-G, Ni-N-G SACs, O-G, and RuO2 tested at 5 mV s-1 and 80% iR correction in 1 mol L?1 KOH. Reprinted with permission from Ref. [52]. Copyright 2020, Wiley-VCH. (d) HAADF-STEM image. Yellow circles represent individually dispersed Fe atoms. (e) C K-edge XAS spectra. The inset spectrum exhibits an enlarged view of the C K-edge XAS spectra ranging from 284 to 290 eV. The inset depicts the structural model of Fe1(OH)x/P-C, where Fe, O, C, and H atoms are represented by blue, red, brown, and white spheres, respectively. (f) Turnover frequencies (TOF) at different overpotentials. (g) Pathway of the OER reaction on Fe1(OH)x/P-C. The Fe, O, C, and H atoms are represented by blue, red, brown, and white spheres, respectively. *OH, *O, and *OOH are the intermediates involved in the OER process. Reprinted with permission from Ref. [53]. Copyright 2021, American Chemical Society.

Fig. 6. (a) LSVs of the Co-N-C were recorded in various KOH solutions with varying concentrations of Fe3+. (b) Spherical aberration-corrected HAADF-STEM images of Co-N-C after activation in Fe-containing KOH (Co-Fe-N-C). XANES spectra (c), K-edge energies (at 50% level) (d) of XANES spectra in panel a and cobalt references compounds containing Co(0), Co(II), or Co(III). (e) Fourier transform of Co K-edge EXAFS spectra without phase correction was performed for as-prepared Co-N-C and the catalyst after activation, as well as during the OER process for different time durations. Reprinted with permission from Ref. [54]. Copyright 2019, American Chemical Society.

Fig. 7. Aberration-corrected HAADF-STEM image (a) and Faradaic efficiency (b) of Fe3+-N-C catalyst. XANES spectra on Fe K-edge (c) and Operando Fe K-edge XANES (d) of Fe3+-N-C catalyst. Reprinted with permission from Ref. [57]. Copyright 2019, AAAS. (e) FE of H2, C1 and C2+ products of N0.14C and Cu/NxC. (f) Scheme of Cun-CuN3 cluster transform in reversible pathway under reaction. Reprinted with permission from Ref. [127]. Copyright 2022, Nature Publishing Group. (g) Difference in theoretical limiting potential for CO2RR and HER for Fe1-N4-C, Fe2-N6-C-p-CO, Fe1-N3-C, Fe2-N6-C-o, and Fe2-N6-C-p. (h) Fe K-edge XANES spectra of different Fex-Ny-C and reference samples. (i) The energy diagram with difference of gibbs free energy on CO2RR for Fe1-N4-C, Fe2-N6-C-o, Fe2-N6-C-p, Fe1-N3-C, and Fe2-N6-C-p-CO. Reprinted with permission from Ref. [129]. Copyright 2022, American Chemical Society. (j) Faradaic efficiency for CO in 0.1 mol L?1 KHCO3 solution on ZIF-NC based samples. (k) The corresponding CO partial current density of the catalysts. Reprinted with permission from Ref. [131]. Copyright 2021, American Chemical Society.

Fig. 8. Scheme of preparing electrocatalysts ZnO3C and ZnN4 (a) and LSV curves of in 0.1 mol L?1 KOH electrolyte (b). (c) The free energy diagram of ZnO3C and ZnN4 towards 2 e- and 4 e- ORR pathway. Reprinted with permission from Ref. [138]. Copyright 2022, Wiley-VCH. (d) Bimetallic Fe-Mn sites was indicated with the intensity profile analysis on TEM result. Fe K-edge XANES (e) and FT-EXAFS spectra (f) of Fe,Mn/N-C and references. LSV curves (g) and Tafel plots (h) of Fe,Mn/N-C, Fe/N-C, Mn/N-C, and Pt/C catalyst in O2-saturated 0.1 mol L-1 HClO4 solution. Reprinted with permission from Ref. [140]. Copyright 2021, Nature Publishing Group.

Fig. 9. (a) Schematic illustration of the synthesis of Fe SAC. (b) FT k3-weighted χ(k)-function of the EXAFS spectra at Fe K-edge. (c) Fitting results of the EXAFS spectra of Fe SAC at k-space. (d) Schematic model of Fe SAC: Fe (yellow), N (blue), and C (gray). (e) LSV curves of the Fe SAC in 0.25 mol L?1 K2SO4 electrolyte and 0.50 mol L?1 KNO3/0.10 mol L?1 K2SO4 mixed electrolyte. (f) NH3 FE of Fe SAC at each given potential. Red dot is FE estimated by three independent NMR tests. (g) NH3 yield rate and partial current density of Fe SAC, FeNP/NC, and NC. Reprinted with permission from Ref. [58]. Copyright 2021, Nature Publishing Group.

Fig. 10. TEM images of AgNP/MnO2 at temperature of 50 °C (a) and 300 °C (b), respectively. (c) HAADF-STEM image of Ag1/MnO2. Reprinted with permission from Ref. [147]. Copyright 2021, Wiley-VCH. In-situ ATR-SEIRAS spectra of Fe1-NC (d) and Fe1-NSC (e) at different applied potentials. Reprinted with permission from Ref. [148]. Copyright 2022, Wiley-VCH. In-situ XAENS spectra (f) and EXAFS profiles (g) of Pd-NC. Reprinted with permission from Ref. [149]. Copyright 2020, Wiley-VCH. In-situ CO DRIFT spectra of Rh single atom based catalyst under CO at increasing temperatures (from bottom to top) (h) and CO DRIFT spectra of Rh single atom based catalyst under CO/O2 at 473?K (i). Reprinted with permission from Ref. [150]. Copyright 2019, Nature Publishing Group.

Fig. 11. (a) In-situ XANES spectra for Ni K-edge of NiFe-CNG with applying different potentials and samples for reference. In-situ FT-EXAFS (b) and WT-EXAFS (c) spectra for Ni K-edge of NiFe-CNG with applying potentials. (d) In-situ XANES spectra for Fe K-edge of NiFe-CNG with applying different potentials and samples for reference. In-situ FT-EXAFS (e) and WT-EXAFS (f) spectra for Fe K-edge of NiFe-CNG with applying potentials. Reprinted with permission from Ref. [151]. Copyright 2021, Nature Publishing Group.

Fig. 12. (a) Operando XANES and (b) FT-EXAFS for Cu K-edge region of Cu/N0.14C from open circuit potential to -1.4?V vs. RHE in 0.1 mol L?1 KHCO3 electrolyte. (c) Absorption edge of Cu/N0.14C was related to the coordination number first shell and second shell with respect to the applied potential. Reprinted with permission from Ref. [127]. Copyright 2022, Nature Publishing Group. (d) XANES spectra at the Mn K-edge of Mn-C3N4/CNT under various reaction conditions Reprinted with permission from Ref. [152]. Copyright 2020, Nature Publishing Group. In-situ Raman spectra (e) and In-situ ATR-SEIRAS (f) of Cu(OH)BTA at the applied potential under CO2 atmosphere and CO2-saturated 0.1? mol L?1 KHCO3 electrolyte, respectively. Reprinted with permission from Ref. [153]. Copyright 2023, Nature Publishing Group.

Fig. 13. Recent trend of publications in single atom catalysts with precious metal elements and non-noble metal elements.

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用于电化学能量转换反应的非贵金属单原子催化剂

Non-noble metal single atom catalysts for electrochemical energy conversion reactions

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