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化学进展 2023, Vol. 35 Issue (6): 821-838 DOI: 10.7536/PC230310 前一篇   后一篇

• 综述 •

单原子催化中的凝聚态化学

李庆贺, 乔波涛*(), 张涛   

  1. 中国科学院大连化学物理研究所催化与新材料研究室 大连 116023
  • 收稿日期:2023-03-13 修回日期:2023-05-18 出版日期:2023-06-24 发布日期:2023-05-25
  • 作者简介:

    乔波涛 中国科学院大连化学物理研究所研究员、“张大煜优秀学 者”。现任《物理化学学报》、Catalysts等期刊编委,《催化学报》青年编委。获2012年首届全国催化新秀奖,2018年“兴辽英才计划青年拔尖人才”。主要研究单原子催化及其在能源转化与环境催化中的应用。在国际期刊上发表论文80余篇, 被引用1万余次。申请发明专利10余件。

  • 基金资助:
    国家重点研发计划(2021YFA1500503); 国家自然科学基金项目(21961142006); 国家自然科学基金项目(21972135); 中国科学院青年基础研究项目(YSBR-022)
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Condensed Matter Chemistry in Single-Atom Catalysis

Qinghe Li, Botao Qiao(), Tao Zhang   

  1. CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China
  • Received:2023-03-13 Revised:2023-05-18 Online:2023-06-24 Published:2023-05-25
  • Contact: *e-mail: bqiao@dicp.ac.cn
  • Supported by:
    The National Key Research and Development Program of China(2021YFA1500503); The National Natural Science Foundation of China(21961142006); The National Natural Science Foundation of China(21972135); The CAS Project for Young Scientists in Basic Research(YSBR-022)

单原子催化,由单原子催化剂推动的催化反应过程,是当前多相催化领域最活跃的研究前沿之一。单原子催化剂是由载体原子与单个金属原子中心通过共价、配位等相互作用,构筑成具有相对明确活性中心的多层次原子聚集体,其组成、结构与性质是凝聚态化学的典型研究对象。本文从凝聚态化学角度出发,简述“单原子催化”概念提出的历史基础和发展现状,系统总结“单原子催化”领域涉及的凝聚态现象即周围原子与金属中心形成的聚集体,详细阐述配位环境对聚集体结构、性质的影响及真实反应状态下聚集体结构动态演变,总结和展望单原子凝聚态效应在多相催化反应领域的应用和未来发展趋势。

关键词： 单原子催化, 聚集体, 凝聚态化学, 结构演变, 原位表征

Single-atom catalysis (SAC), the catalysis by single-atom catalysts (SACs), has been developed as one of the most active research frontiers in the field of heterogeneous catalysis. SACs are multilevel atomic aggregates with relatively clear active center consisting of single metal atoms stabilized on support atoms through covalent or coordination interaction. Their composition, structure and properties are typical research objects of condensed matter chemistry. This review paper starts from the view of condensed matter chemistry and the main contents are as follows: briefly describing the historical basis and development status of the concept of SAC; systematically summarizing the condensed matter phenomena involved in the field of SAC, that's the aggregate of the surrounding atoms and the metal center; elaborating the influence of coordination environment on the structure and properties of aggregates and the dynamic evolution of aggregate structure under real reaction condition. Finally, the application and future development trend of condensed matter effect of single atom in heterogeneous catalytic reactions are summarized and prospected.

Contents

1 Introduction

2 The concept of "single atom catalysis"

3 The development of "single atom catalysis"

3.1 Preparation of single atom catalyst

3.2 Characterization of single atom catalyst

3.3 Application of single atom catalyst

4 Condensation effect between metal center and coordination atoms

4.1 Interaction form between metal and support

4.2 Aggregates structure modulating via coordination atoms

4.3 Effect of metal aggregation form on catalytic performance

5 Dynamic evolution and characterization of aggregates under reactive conditions

6 Conclusion and outlook

Key words: single-atom catalysis, aggregation, condensed matter chemistry, structural evolution, in-situ characterization
()
图1 “单原子催化”概念提出
Fig.1 Proposing the concept of "single atom catalysis"
图2 “单原子催化”发展历程[27]
Fig.2 The development of "single-atom catalysis"[27]. Copyright 2020, Springer
图3 制备SACs的多种宿主材料[71]
Fig.3 Various host materials for preparation of SACs[71]. Copyright 2018, Wiley
表1 单原子催化剂不同制备方法对比
Table 1 Comparison of the different preparation methods for SACs
分类 方法名称 优点 缺点
自下而上 质量分离软着陆法 原子分布均匀 需要特殊设备、反应条件苛刻、成本高
原子层沉积法
球磨法 成本低、操作简便 小球或添加剂的污染
湿化学法 制备过程简便、无需特殊复杂设备
电沉积法 精确控制原子分散 电解质溶液可能引入杂质,金属单原子与载体的作用力不可控,对金属物种还原电位有特殊要求
自上而下 高温热解法 热稳定性高 成本高
表2 单原子催化剂表征方法
Table 2 Characterization methods for SACs
表征方法 简写 特点 结构信息
1 透射电子显微镜 TEM 直观、可视性;检测区域具有限制性,无法反映样品的整体信息 催化剂原子尺度信息
2 扫描透射显微镜 STEM 通过机械操作导电尖端,记录隧穿电流,对表面原子位置进行常规成像 催化剂原子尺度信息
3 X 射线光电子能谱 XPS 表面信息 揭示单原子催化剂表面化学组成和原子价态信息
4 红外光谱技术 IR 仪器和操作简单;能够方便、 快速且经济地提供位点特异性信息 催化剂金属原子分散性质,推断出活性中心及其局部结构特征
5 X射线吸收光谱 XAS 分辨率高、可在原位条件下操作 提供高灵敏度的宏观平均结构特征和配位信息
6 电子自旋共振 EPR 用于探测含有未配对电子的顺磁性物种 可提供顺磁中心的性质:对称性、电子结构、价态变化以及与反应物的相互作用等
7 核磁共振 NMR 确定金属原子的锚定位点、跟踪有机金属前驱体的吸附情况 提供单原子催化剂的结构信息
8 低能离子散射谱 LEIS 对被测元素最外层原子敏感 有助于定性分析目标原子表面分布,或进一步对其浓度定量
图4 单原子催化剂聚集体构型(a)正四面体(b)平面四边形(c和d)正八面体
Fig.4 Aggregate configurations of SACs (a) tetrahedron, (b) Plane quadrilateral, (c) and (d) regular octahedron
表3 金属单原子(M)在载体(Sup)上锚定位置列表[19]
Table 3 A list of the anchoring positions of metal single atoms (M) on the support (Sup)[19]. Copyright 2020, ACS
Sup
M CeO2 FeOx Al2O3 TiO2 WOx MgO ZnO MnO2
Co D,Mv
Ni Mv
Cu Ov Mv
Ru Al3+ Mv
Pd D D D,Ov
Ag Mv
Pt D,Ov Ov,Mv Al3+ D,Ov,
Mv,Ti3+		 Ov Mv
Au Ov, Mv Mv Ov Mv Mv
Mo Mv
图5 Pt1/TiO2催化剂原位CO-DRIFT谱图[107]
Fig.5 In situ CO-DRIFT spectra of Pt1/TiO2 catalyst[107]. Copyright 2020, Wiley
图6 Pt在不同载体上的烧结与分散[109]
Fig.6 Sintering and dispersion of Pt on different supports[109]. Copyright 2019, Springer
图7 纳米颗粒、团簇和单原子的(a)几何结构与(b)电子结构[24]
Fig.7 (a) Geometric and (b) electronic structures of nanoparticles, clusters and single atoms[24]. Copyright 2018, ACS
图8 CeO2负载的Ru单原子、团簇以及纳米颗粒的甲烷化活性对比[125]
Fig.8 Comparison of methanation activity of Ru single-atoms, clusters and nanoparticles supported on CeO2[125]. Copyright 2018, ACS
图9 In2O3负载的Re单原子、团簇以及纳米颗粒的CO2加氢产物选择性[127]
Fig.9 CO2 hydrogenation product selectivity of Re single-atoms, clusters and nanoparticles supported on In2O3[127]. Copyright 2022, ACS
图10 包裹纳米颗粒暴露单原子调控加氢产物选择性。乙炔半加氢反应中不同还原温度处理的催化剂(Pd/TiO2-H200,Pd单原子和Pd纳米颗粒共存;Pd/TiO2-H600,Pd纳米颗粒被包裹,Pd单原子为活性中心)的(a)C2H2转化率和(b)C2H4选择性[128]
Fig.10 Encapsulation nanoparticles while exposing single atoms to regulate hydrogenation product selectivity. Semi-hydrogenation of acetylene (a) The C2H2 conversion and (b) C2H4 selectivity of catalysts treated at different reduction temperatures (Pd/TiO2-H200: contains Pd single-atoms and Pd nanoparticles; Pd/TiO2-H600: Pd nanoparticles are encapsulated while exposing Pd single-atoms as the active center)[128]. Copyright 2022, Springer
图11 Co-N-C单原子催化剂形貌、组成及结构分析[132]
Fig.11 Morphology, composition and structure analysis of Co-N-C SACs[132]. Copyright 2016, Wiley
图12 SAA表征方法:(a,b)Pt1Cu SAA催化剂的 HAADF-STEM图像,Pt1Sn SAA催化剂的(c)Pt-L3 edge XANES 和 (d) Pt 4f XPS谱[139]
Fig.12 The characterizations of SAA. (a,b) HAADF-STEM images of Pt1Cu catalyst, (c) Pt-L3 edge XANES and (d) XPS Pt 4f spectra for Pt1Sn SAA[139]. Copyright 2018, Springer
图13 铜单原子催化剂在N2电化学还原反应中结构变化[146]
Fig.13 Structural changes of Cu SACs during the electrochemical reduction of N2[146]. Copyright 2018, ACS
图14 铜单原子催化剂在O2电化学还原反应中结构变化[147]
Fig.14 Structural changes of Cu SACs during the electrochemical reduction of O2[147]. Copyright 2021, ACS
图15 Cu单原子和团簇之间的可逆转变[148]
Fig.15 Reversible transition between Cu single-atoms and clusters[148]. Copyright 2022, ACS
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摘要

单原子催化中的凝聚态化学