纳米催化剂的理性设计与精准调控

doi:10.1016/S1872-2067(21)63933-5

催化学报 ›› 2022, Vol. 43 ›› Issue (4): 898-912.DOI: 10.1016/S1872-2067(21)63933-5

纳米催化剂的理性设计与精准调控

刘清港, 马俊国, 陈晨^*()

清华大学化学系, 北京100084

收稿日期:2021-07-29 接受日期:2021-07-29 出版日期:2022-03-05 发布日期:2021-09-06
通讯作者: 陈晨
基金资助:
国家重点研发计划(2016YFA0202801);国家重点研发计划(2017YFA0700101);国家自然科学基金(21925202);国家自然科学基金(21872076);国家自然科学基金(22008136);北京自然科学基金(JQ18007);清华大学自主科研计划资助

Rational design and precise manipulation of nano-catalysts

Qinggang Liu, Junguo Ma, Chen Chen^*()

Department of Chemistry, Tsinghua University, Beijing 100084, China

Received:2021-07-29 Accepted:2021-07-29 Online:2022-03-05 Published:2021-09-06
Contact: Chen Chen
About author:Chen Chen received his BS degree from the Department of Chemistry, Beijing Institute of Technology in 2006, and his PhD degree from the Department of Chemistry, Tsinghua University in 2011. After the postdoctoral work at Lawrence Berkeley National Laboratory, he joined the Department of Chemistry at Tsinghua University as an Associate Professor in 2015, and was promoted to Professor with tenure in 2021. His research interests are focused on nanomaterials for catalysis and sustainable energy. His name is in the lists of Highly Cited Researchers 2021 from Clarivate. He joined the Editorial Board of Chinese Journal of Catalysis in 2020.
Supported by:
National Key R&D Program of China(2016YFA0202801);National Key R&D Program of China(2017YFA0700101);National Natural Science Foundation of China(21925202);National Natural Science Foundation of China(21872076);National Natural Science Foundation of China(22008136);Beijing Natural Science Foundation(JQ18007);Tsinghua University Initiative Scientific Research Program

摘要/Abstract

摘要：

纳米催化在现代化学工业中起着至关重要的作用. 当前社会的高速发展, 促使人们在不同领域探索新型纳米催化剂引导技术革命以解决日益严峻的能源及环境危机. 要实现在原子水平上精确调控并对催化剂结构进行设计以开发高效的纳米催化剂, 必须深入了解其中的基本物理化学理论, 如活性中心的配位结构以及催化剂与吸附质之间的作用规律等. 然而, 受当前表征技术和理论化学及合成方法学的限制, 从复杂的纳米催化体系中剥离出真正的活性位并对其进行精确定向合成还面临极大的挑战. 本文总结了影响纳米催化的因素, 并重点阐述了开发电催化和光催化及热催化纳米催化剂中涉及的合成策略.
在电催化反应体系中, 围绕电解水和氢燃料电池以及CO₂电还原催化剂的开发策略进行了阐述. 为缓解当前商用析氢和析氧催化剂对贵金属的依赖, 本课题组基于具有核壳结构的金属-有机聚合物前体开发了一种热解策略, 分别制备了多孔氮掺杂碳材料包覆的CoP/NCNHP和MoP@NCHSs电解水催化剂. 得益于多孔碳材料暴露的高活性位数量及氮物种与活性金属之间的强协同作用, 该类催化剂在催化酸性析氢反应(HER)和碱性HER以及析氧反应(OER)中表现出高效的活性和稳定性. 此外, 本文介绍了一种可以极大提高金属利用效率的Pt₃Ni纳米框架催化剂. 该框架结构呈现独特的Pt表面富集特征, 不仅最大限度地暴露了高活性的棱/角位点, 还有利于分子在框架内部的扩散传质, 这种独特的结构使其在氧还原反应(ORR)中表现出较好的催化活性. 针对电催化CO₂还原, 本文重点阐述了氮配位策略在单原子催化中的应用, 并针对单原子在催化多分子转化时面临的挑战, 发展了一种“原子对”催化剂.
在光催化反应体系中, 为促进光生电子-空穴对的分离并抑制其复合, 本课题组报道了一种具备快速可逆光致变色能力的Bi₂WO_6‒_x纳米片. 与传统光致变色材料不同, Bi₂WO_6‒_x纳米片在光照及O₂的作用下可以实现光生电子的快速利用及空穴的消耗, 使光生载流子分离得到显著而持续的增强; 此外, 通过比较载流子在不同晶面的动力学差异, 本课题组还揭示了少数载流子动力学对光催化反应活性的影响规律, 实现了温和条件下光催化高效碳氢键活化.
在多相催化反应体系中, 总结了一系列控制金属原子聚集状态的制备策略. 针对工业上重要的硅烷氧化和苯氧化以及N-甲酰化反应, 重点阐述了氮配位及MXene缺陷稳定策略在制备单原子Au₁/mpg-C₃N₄、Fe-N₄以及Pt₁/Ti_3‒_xC₂T_y催化剂中的应用及反应活性位点的调控研究.

关键词: 纳米催化, 单原子催化剂, 水分解, 氧还原反应, CO₂还原反应, 硅烷氧化, 苯氧化, N-甲酰化

Abstract:

Nano-catalysis plays a vital role in the chemical transformations and significantly impacts the booming modern chemical industry. The rapid technological enhancements have resulted in serious energy and environmental issues, which are currently spurring the exploration of the novel nano-catalysts in diverse fields. In order to develop the efficient nano-catalysts, it is essential to understand their fundamental physicochemical properties, including the coordination structures of the active centers and substrate-adsorbate interactions. Subsequently, the nano-catalyst design with precise manipulation at the atomic level can be attained. In this account, we have summarized our extensive investigation of the factors impacting nano-catalysis, along with the synthetic strategies developed to prepare the nano-catalysts for applications in electrocatalysis, photocatalysis and thermocatalysis. Finally, a brief conclusion and future research directions on nano-catalysis have also been presented.

Key words: Nano-catalysis, Single-atom catalysts, Water splitting, Oxygen reduction reaction, CO₂ reduction reaction, Silane oxidation, Benzene oxidation, N-formylation

刘清港, 马俊国, 陈晨. 纳米催化剂的理性设计与精准调控[J]. 催化学报, 2022, 43(4): 898-912.

Qinggang Liu, Junguo Ma, Chen Chen. Rational design and precise manipulation of nano-catalysts[J]. Chinese Journal of Catalysis, 2022, 43(4): 898-912.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)63933-5

https://www.cjcatal.com/CN/Y2022/V43/I4/898

图/表 11

Fig. 1. Overview of the topics covered in this account.

Fig. 2. (a) Schematic illustration of the preparation for the CoP/NCNHP; (b) The linear sweep voltammetry (LSV) curve of the CoP/NCNHP// CoP/NCNHP electrode in 1 mol/L KOH with iR compensation in a two-electrode system; (c) Chronopotentiometric curve of water electrolysis at different current densities in 1 mol/L KOH; (d) Calculated density of states (DOS) for CoP/NCNHP and pure CoP; (e) Charge density distribution maps of the CoP/NCNHP catalyst; (f) Calculated free energy diagram of the HER on CoP, surface-oxidized 50% CoP, and surface-oxidized 100% CoP, respectively. Reprinted with permission from Ref. [73]. Copyright 2018, American Chemical Society.

Fig. 3. (a) LSV curves of MoP@NCHSs-T, bulk MoP, and commercial 20% Pt/C in 1.0 mol/L KOH; (b) Stability of the MoP@NCHSs-900 catalyst in 1.0 mol/L KOH; (c) Average Bader charge of N-doping carbon; (d) Free energy diagram of the water dissociation step. Reprinted with permission from Ref. [74]. Copyright 2019, John Wiley and Sons.

Fig. 4. (a) Schematic illustrations and corresponding TEM images of the samples during the evolution process from polyhedral to nanoframes; (b) HAADF-STEM image and corresponding EDX data (mapping and line-scan) of annealed hollow Pt3Ni nanoframe; (c) Specific activities measured at 0.95 V, and improvement factors versus Pt/C catalysts; (d) ORR polarization curves and corresponding Tafel plots (inset) of Pt3Ni frames before and after 10000 potential cycles. Reprinted with permission from Ref. [80]. Copyright 2014, American Association for the Advancement of Science.

Fig. 5. (a) Schematic illustration of the preparation for the Co-N5/HNPCSs catalyst; (b) HAADF-STEM and EDS images of the Co-N5/HNPCSs catalyst; LSV curves (c) and FECO and FEH2 (d) of the Co-N5/HNPCSs and CoPc catalysts; (e) Calculated free energy of CO2RR. Reprinted with permission from Ref. [82]. Copyright 2018, American Chemical Society.

Fig. 6. (a) Current-voltage curves for different samples from LSV scans; (b) FECO and FEH2 of different Cu-loaded samples at -0.78 V (vs. RHE); (c) Free energy profiles for CO2 activation on Cu, Cu@Cu2O and Cu-APC. (d) Configurations of physisorbed CO2 and chemisorbed CO2 on Cu-APC. Reprinted with permission from Ref. [83]. Copyright 2019, Springer Nature.

Fig. 7. (a) Schematic illustration of photoinduced hole on {110} and {001} of WO3 during BA oxidation. (b) Morphology model and HRTEM graph of WO3 nanowire and nanosheet. Dynamics of carriers on two crystal facets: hole mobility (c); electron mobility (d); hole diffusion length (e); reaction rates of benzyl alcohol oxidation (f); steady state fluorescence (g); and hole lifetime (h). Reprinted with permission from Ref. [90]. Copyright 2018, American Chemical Society.

Fig. 8. (a) Schematic illustration of the structure and catalytic mechanism of p-BWO; (b) TEM image of the p-BWO nanosheets; (c) Digital photographs of p-BWO in the initial versus coloured state; (d) Photoluminescence emission spectra (excitation at 340 nm) of the p-BWO and pristine Bi2WO6; (e) Conversion rate of toluene oxidation for Bi2WO6 and p-BWO with different substrate loadings; (f) Schematic of the separation of photoinduced carriers of p-BWO, and the mechanism of photocatalytic reaction and photochromism. Reprinted with permission from Ref. [93]. Copyright 2019, Springer Nature.

Fig. 9. (a) The aberration-corrected HAADF-STEM images of Au1/mpg-C3N4; (b) Fourier transform magnitudes of the EXAFS spectra for Au1/mpg-C3N4, Au NPs/mpg-C3N4 and Au foil; (c) Conversion rate of the diphenylmethylsilane in water with different Au catalysts; (d) The mechanism of silane oxidation over single-site Au catalyst. Reprinted with permission from Ref. [99]. Copyright 2018, John Wiley and Sons.

Fig. 10. The aberration-corrected HAADF-STEM images of the Fe-N4 SAs/N-C (a), Fe-N3C1 SAs/N-C (b), FeN2C2 SAs/N-C (c) catalysts. The insets are the corresponding structure model. (d) HAADF-STEM-EDS mapping of the Fe-N4 SAs/N-C catalyst; XANES spectra at the C K-edge (e), N K-edge (f), and Fe L-edge (g). Reprinted with permission from Ref. [103]. Copyright 2019, Springer Nature.

Fig. 11. (a) Illustration of the self-reduction method for the preparation of Pt1/Ti3-xC2Ty; (b) HAADF-STEM image of Pt1/Ti3-xC2Ty and corresponding intensity maps obtained in line 1 in (b); (c) Catalytic performance of the N-formylation of aniline using different catalysts and the recycling test of Pt1/Ti3-xC2Ty; (d) EXAFS spectra of Pt1/Ti3-xC2Ty; (e) Charge density difference of Pt1/Ti3-xC2Ty with a plain view. Reprinted with permission from Ref. [107]. Copyright 2019, American Chemical Society.

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纳米催化剂的理性设计与精准调控

Rational design and precise manipulation of nano-catalysts

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