超高选择性CO2光还原为乙醇的CuNi异核双原子催化剂的精准设计

doi:10.1016/S1872-2067(23)64630-3

催化学报 ›› 2024, Vol. 59: 126-136.DOI: 10.1016/S1872-2067(23)64630-3

超高选择性CO₂光还原为乙醇的CuNi异核双原子催化剂的精准设计

崔恩田^a, 鲁玉莲^a, 江吉周^b^,^*(), 王定胜^e, 翟天佑^c

^a盐城工学院江苏省新型环保重点实验室, 江苏盐城224051, 中国
^b武汉工程大学环境生态与生物工程学院, 湖北新型催化材料工程研究中心, 教育部磷资源开发利用工程研究中心, 教育部绿色化工过程重点实验室, 湖北武汉430205, 中国
^c清华大学化学系, 北京100084, 中国
^d华中科技大学材料科学与工程学院材料加工与模具技术国家重点实验室, 湖北武汉430074, 中国
^e印尼纳米中心, 万丹, 印尼

收稿日期:2023-12-29 接受日期:2024-02-07 出版日期:2024-04-18 发布日期:2024-04-15
通讯作者: *电子信箱: 027wit@163.com (江吉周).
基金资助:
国家自然科学基金(62004143);湖北省重点研发计划(2022BAA084)

Tailoring CuNi heteronuclear diatomic catalysts: Precision in structural design for exceptionally selective CO₂photoreduction to ethanol

Entian Cui^a, Yulian Lu^a, Jizhou Jiang^b^,^*(), Arramel ^e, Dingsheng Wang^c, Tianyou Zhai^d

^aKey Laboratory for Advanced Technology in Environmental Protection of Jiangsu Province, Yancheng Institute of Technology, Yancheng 224051, Jiangsu, China
^bSchool of Environmental Ecology and Biological Engineering, School of Chemistry and Environmental Engineering, Key Laboratory of Green Chemical Engineering Process of Ministry of Education, Engineering Research Center of Phosphorus Resources Development and Utilization of Ministry of Education, Novel Catalytic Materials of Hubei Engineering Research Center, Wuhan Institute of Technology, Wuhan 430205, Hubei, China
^cDepartment of Chemistry, Tsinghua University, Beijing 100084, China
^dState Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, Hubei, China
^eNano Center Indonesia, Jalan Raya PUSPIPTEK, South Tangerang, Banten 15314, Indonesia

Received:2023-12-29 Accepted:2024-02-07 Online:2024-04-18 Published:2024-04-15
Contact: *E-mail:027wit@163.com (J. Jiang).
Supported by:
The National Natural Science Foundation of China(62004143);The Key R&D Program of Hubei Province(2022BAA084)

摘要/Abstract

摘要：

利用光催化还原技术将CO₂定向转化为乙醇(CO₂-乙醇)是解决日益严重的环境污染和能源危机的理想途径之一. 然而, CO₂分子的高化学惰性以及C-C耦合反应的高化学能垒导致目前CO₂-乙醇转化反应的产率和选择性较低. 因此, 设计构建能够快速活化CO₂分子并同时促进C-C耦合的光催化材料具有重要研究意义. 尽管已有研究表明, Cu⁺物种在促进C-C耦合方面具有一定优势, 但其在催化反应过程中的不稳定性限制了其实际应用.

基于上述认识, 本文通过理论模拟预测发现, 相比于Cu单原子, CuNi异核双原子(CuNi HDAs)不仅在CO₂活化及C-C耦合方面更具优势, 而且能够有效锚定并固化Cu⁺物种. 因此, 本文设计了一种三步合成策略, 精准地将Cu单原子锚定在(Ni, Zr)-UiO-66-NH₂材料的Ni位上, 合成了以CuNi HDAs为活性位点的Cu-(Ni, Zr)-UiO-66-NH₂光催化材料. 在可见光照射下, Cu-(Ni, Zr)-UiO-66-NH₂表现出较好的催化CO₂-乙醇转化活性, 其乙醇的产率和选择性分别达到~3218 μmol·g_Cu^-1·h^-1和97.3%. 光谱分析和密度泛函理论计算结果表明, Cu-(Ni, Zr)-UiO-66-NH₂材料较好的光催化性能来源于CuNi HDAs特殊的电子结构. 首先, CuNi HDAs通过CuNi-O界面化学键与吸光组分(Ni, Zr)-UiO-66-NH₂相连, 利用界面Cu-Ni-O键作为快速电子传输通道, CuNi HDAs能够富集到足够的光生电子用于涉及12电子的CO₂-乙醇转化反应, 使得乙醇产率大幅提升. 其次, Cu, Ni和O三种原子由于电子亲核能的差异, 导致CuNi HDAs的电子分布呈现不对称性. 这种不对称的电子结构能有效诱导CO₂分子的极化, 打破其结构的对称性, 从而显著降低CO₂分子的活化能. 再次, 相比于Cu单原子, CuNi HDAs对*CO中间体的吸附能力更强, 这不仅增强了活性位点表面*CO中间体的覆盖度, 还抑制CO的生成, 为C-C耦合创造了充分条件. 最后, 由于Cu-Ni双活性位电子密度的差异, CuNi HDAs表面的C-C耦合反应势能较低, 有利于*OCCHO中间体的快速生成, 从而使乙醇产物的选择性大幅提升.

综上, 本文以理论计算模拟为指导, 以UiO-66-NH₂材料为基底, 成功设计并制备了一种具有不对称电子结构的CuNi HDAs光催化材料, 实现了高选择性CO₂光还原为乙醇. 研究表明, CuNi HDAs的不对称结构在促进分子活化和降低C-C耦合反应能垒中起关键作用, 同时促进了光生电子在CuNi HDAs活性位的富集. 本文的研究结果为在原子尺度上设计并合成高性能的CO₂还原光催化剂提供了实验和理论参考.

关键词: CuNi异核双原子, 光催化, CO₂-乙醇转化, 不对称电子分配, 电子富集

Abstract:

The photocatalytic reduction of CO₂to ethanol has attracted extensive attention, particularly for intricate C-C coupling. In this study, we propose a synthetic pathway for asymmetric CuNi heteronuclear diatoms (CuNi HDAs) by anchoring single Cu atoms on the Ni sites of (Ni, Zr)-UiO-66-NH₂ to enhance C-C coupling. Cu-(Ni,Zr)-UiO-66-NH₂ efficiently performs photocatalytic CO₂ conversion with a mass-specific activity (selectivity) of 3218 μmol·g_Cu^-1·h^-1 (97.3%). Spectroscopic analyses and density functional theory calculations revealed that CuNi HDAs with an asymmetric electronic distribution facilitated the activation of CO₂ molecules and lowered the C-C coupling barrier energy, thus promoting the formation of *OCCHO intermediates. This, in turn, led to a significant enhancement of ethanol selectivity. Furthermore, with interfacial Cu-Ni-O bonds as a rapid electron transport channel, CuNi HDAs enrich enough electrons for 12-electron CO₂ reduction, thereby enhancing ethanol productivity. This study provides a novel strategy for designing highly selective photocatalysts for CO₂ conversion at the atomic scale.

Key words: CuNi heteronuclear diatoms, Photocatalysis, CO₂-to-ethanol conversion, Asymmetric electronic distribution, Electron enrichment

崔恩田, 鲁玉莲, 江吉周, 王定胜, 翟天佑. 超高选择性CO₂光还原为乙醇的CuNi异核双原子催化剂的精准设计[J]. 催化学报, 2024, 59: 126-136.

Entian Cui, Yulian Lu, Jizhou Jiang, Arramel , Dingsheng Wang, Tianyou Zhai. Tailoring CuNi heteronuclear diatomic catalysts: Precision in structural design for exceptionally selective CO₂photoreduction to ethanol[J]. Chinese Journal of Catalysis, 2024, 59: 126-136.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(23)64630-3

https://www.cjcatal.com/CN/Y2024/V59/I4/126

图/表 5

Fig. 1. (a) Structure of Cu-(Ni,Zr)-UiO-66-NH2. (b) Gibbs free energy difference between C-C coupling and *CO protonation on UiO-66-NH2, (Ni,Zr)-UiO-66-NH2, and Cu-(Ni,Zr)-UiO-66-NH2. (c) Geometries of *CO, *CHO, and *OCCHO intermediates on Cu-(Ni,Zr)-UiO-66-NH2. (d,e) Charge density difference distribution and ELF of UiO-66-NH2, (Ni, Zr)-UiO-66-NH2, and Cu-(Ni,Zr)-UiO-66-NH2.

Fig. 2. (a) Schematic diagram of the synthesis. TEM image (b), EDS mapping (c), STEM image (d), Cu K-edge XANES spectra (e), Ni K-edge XANES spectra (f), Cu K-edge EXAFS spectra (g), Ni K-EXAFS spectra (h), Ni 2p (i), and Cu 3d (j) XPS spectra of Cu-(Ni, Zr)-UiO-66-NH2.

Fig. 3. (a,b) Comparative production and selectivity of CH3OH and CH3CH2OH on different photocatalysts. (c) MS spectra of 13C and 12C liquid products from the 13CO2 and 12CO2 photoreduction products, respectively, of Cu-(Ni,Zr)-UiO-66-NH2. Cyclic activity tests (d), diffuse reflectance spectra (e), photocurrent plots (f), Nyquist plots of EIS (g), PL (h), and time-resolved fluorescence spectra (i) of Cu-(Ni,Zr)-UiO-66-NH2.

Fig. 4. 2D mapping of TA spectra, TA spectra signals, and normalized decay kinetic curves of UiO-66-NH2 (a-c), (Ni,Zr)-UiO-66-NH2 (d-f), and Cu-(Ni, Zr)-UiO-66-NH2 (g-i).

Fig. 5. Cu 2p in-situ XPS spectra (a) and Ni 2p in-situ XPS spectra (b). In-situ FT-IR spectra (c) and corresponding mapping result (d), TDOS plots (e), PDOS plots (f). Calculated adsorption energy of CO on Cu-(Ni,Zr)-UiO-66-NH2 (g) and free energy diagram (h) of the mechanism of CO2 reduction.

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超高选择性CO₂光还原为乙醇的CuNi异核双原子催化剂的精准设计

Tailoring CuNi heteronuclear diatomic catalysts: Precision in structural design for exceptionally selective CO₂photoreduction to ethanol

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