通过双活化策略在Ag-CeO2电催化剂上用苯乙酮高效固定CO2

doi:10.1016/S1872-2067(22)64116-0

催化学报 ›› 2022, Vol. 43 ›› Issue (12): 3134-3141.DOI: 10.1016/S1872-2067(22)64116-0

通过双活化策略在Ag-CeO₂电催化剂上用苯乙酮高效固定CO₂

关安翔^a^,^†, 全粤莉^a^,^†, 陈杨屾^a, 刘铮铮^a, 张俊波^a, 阚淼^a, 张全^a, 黄浩量^b, 钱林平^a, 张林娟^b, 郑耿锋^a^,^*()

^a复旦大学先进材料实验室, 复旦大学化学系和上海市分子催化与创新材料重点实验室, 上海200438
^b中国科学院上海应用物理研究所界面物理与技术重点实验室, 上海201800

收稿日期:2022-03-29 接受日期:2022-04-27 出版日期:2022-12-18 发布日期:2022-10-18
通讯作者: 郑耿锋
作者简介:第一联系人：
^†共同第一作者.
基金资助:
国家重点研发项目(2018YFA0209401);国家自然科学基金(22025502);国家自然科学基金(21975051);上海市科学技术委员会资助项目(21DZ1206800);上海市教育委员会创新项目(2019-01-07-00-07-E00045)

Efficient CO₂ fixation with acetophenone on Ag-CeO₂ electrocatalyst by a double activation strategy

Anxiang Guan^a^,^†, Yueli Quan^a^,^†, Yangshen Chen^a, Zhengzheng Liu^a, Junbo Zhang^a, Miao Kan^a, Quan Zhang^a, Haoliang Huang^b, Linping Qian^a, Linjuan Zhang^b, Gengfeng Zheng^a^,^*()

^aLaboratory of Advanced Materials, Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis & Innovative Materials, Fudan University, Shanghai 200438, China
^bKey Laboratory of Interfacial Physics and Technology, Shanghai Institute of Applied Physics, Chinese Academy of Sciences, Shanghai 201800, China

Received:2022-03-29 Accepted:2022-04-27 Online:2022-12-18 Published:2022-10-18
Contact: Gengfeng Zheng
About author:First author contact:^†Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2018YFA0209401);National Natural Science Foundation of China(22025502);National Natural Science Foundation of China(21975051);Science and Technology Commission of Shanghai Municipality(21DZ1206800);Shanghai Municipal Education Commission(2019-01-07-00-07-E00045)

摘要/Abstract

摘要：

二氧化碳(CO₂)是一种主要的温室气体, 对全球气候变化和生态环境造成了很大影响. 同时, CO₂也是一种无毒、廉价、丰富的C₁资源, 可用于合成用作燃料和药物的各种有机化合物. 因此, 模拟植物光合作用对CO₂进行固定成为了众多科研工作者的研究热点. 电化学羧化是将CO₂固定在有机分子上的一种有效方法, 并且已被证明可以通过构建新的C-C键, 使CO₂与各种底物(包括酮、二烯和类卤化物等)发生电羧化反应, 形成羧酸化合物. 然而, 由于CO₂分子本身的热力学和动力学惰性, 使得CO₂分子的活化颇具挑战性, 难以实现高效转化. 目前, 许多研究致力于开发各种用于CO₂转化的反应模型和催化剂. 例如, 结合单个CO₂分子形成不同羧酸的单羧基化反应. 酮类化合物与CO₂的电羧化反应是实现CO₂固定并合成羧酸的一种有效途径, 得到的羧酸产物可作为许多生物活性化合物的来源. 然而, 在CO₂和芳香酮的电羧化反应中, 由于二者的活化具有较大的过电位差异, 会严重阻碍电羧化反应的效率并导致产物收率较低. 研究表明可以通过同时激活CO₂分子和有机底物以促进目标羧化产物的形成. 该策略为改善CO₂和芳族酮之间的电羧化反应效率提供了思路.

本文合成了一种Ag掺杂的CeO₂纳米线(Ag-CeO₂ NWs)作为催化苯乙酮和CO₂进行电羧化反应的催化剂. 该催化剂能够起到同时活化CO₂和苯乙酮分子的作用, 实现双重活化的目的. 在双重活化策略下, 苯乙酮与CO₂的电羧化反应可以通过将CO₂活化为CO₂^•-, 然后通过自由基的形式加成到苯乙酮的双键上; 或者, 苯乙酮分子被活化成苯乙酮自由基阴离子, 苯乙酮自由基阴离子通过亲核反应与CO₂偶联, 最终形成羧酸产物. 与银箔、银纳米颗粒和CeO₂纳米线相比, Ag-CeO₂纳米线催化剂可以有效降低CO₂和苯乙酮分子活化之间的起始电位差, 从而能够有效地电羧化形成2-苯乳酸. 在-1.8 V vs. Ag/AgI电位下, 生成2-苯乳酸的法拉第效率高达91%, 收率为83.2%. 综上, 本文同时激活CO₂和有机底物分子的双重活化策略有利于指导催化剂的设计, 从而提高CO₂固定效率, 进而提高电羧化反应的活性和选择性.

关键词: 电羧化反应, 二氧化碳还原, 电催化剂, Ag-CeO₂, 双重活化策略

Abstract:

The electrocarboxylation reaction is an attractive means to convert CO₂ into valuable chemicals under ambient conditions, while it still suffers from low efficiency due to the high stability of CO₂. In this work, we report a double activation strategy for simultaneously activating CO₂ and acetophenone by silver-doped CeO₂ (Ag-CeO₂) nanowires, featuring as an effective electrocatalyst for electrocarboxylation of acetophenone with CO₂. Compared to the Ag foil, Ag nanoparticles and CeO₂ nanowires, the Ag-CeO₂ nanowire catalyst allowed to reduce the onset potential difference between CO₂ and acetophenone activation, thus enabling efficient electrocarboxylation to form 2-phenyllactic acid. The Faradaic efficiency for producing 2-phenyllactic acid reached 91% at -1.8 V versus Ag/AgI. This double activation strategy of activating both CO₂ and organic substrate molecules can benefit the catalyst design to improve activities and selectivities in upgrading CO₂ fixation for higher-value electrocarboxylation.

Key words: Electrocarboxylation, CO₂ reduction, Electrocatalyst, Ag-CeO₂, Double activation strategy

关安翔, 全粤莉, 陈杨屾, 刘铮铮, 张俊波, 阚淼, 张全, 黄浩量, 钱林平, 张林娟, 郑耿锋. 通过双活化策略在Ag-CeO₂电催化剂上用苯乙酮高效固定CO₂[J]. 催化学报, 2022, 43(12): 3134-3141.

Anxiang Guan, Yueli Quan, Yangshen Chen, Zhengzheng Liu, Junbo Zhang, Miao Kan, Quan Zhang, Haoliang Huang, Linping Qian, Linjuan Zhang, Gengfeng Zheng. Efficient CO₂ fixation with acetophenone on Ag-CeO₂ electrocatalyst by a double activation strategy[J]. Chinese Journal of Catalysis, 2022, 43(12): 3134-3141.

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图/表 5

Fig. 1. Schematic illustration of the synthesis procedure for the Ag-CeO2 NWs and the electrocarboxylation between acetophenone and CO2.

Fig. 2. (a) XRD patterns of CeO2 NWs (blue curve) and Ag-CeO2 NWs (red curve). (b) SEM image of Ag-CeO2 NWs. TEM (c) and high-resolution TEM (d) images of Ag-CeO2 NWs. (e) EDS elemental mapping of Ag-CeO2 NWs.

Fig. 3. XPS spectra of Ag-CeO2 NWs in the Ce 3d (a) and Ag 3d (b) regions. (c) XANES spectra of Ag K-edge for Ag-CeO2 NWs (red curve) and Ag foil (black curve). (d) First-derivatives of the XANES region for Ag-CeO2 NWs (upper panel) and Ag foil (low panel). (e) Wavelet-transform images of EXAFS data at Ag K-edge for Ag foil (upper panel) and Ag-CeO2 NWs (lower panel). (f) FT-EXAFS spectra of Ag K-edge for Ag-CeO2 NWs (red curve) and Ag foil (black curve).

Fig. 4. (a) Linear sweep voltammetry curves for Ag-CeO2 NWs sample in anhydrous acetonitrile with 0.2 mol L?1 tetrabutylammonium bromide under different reaction conditions: CO2 only (blue curve); acetophenone only (orange curve); and both CO2 and acetophenone (red curve). (b) Partial current densities (upper panel) and Faradaic efficiencies (lower panel) of 2-phenyllactic acid at different applied potentials when using the Ag-CeO2 NWs as catalyst. (c) Partial current densities (upper panel) and Faradaic efficiencies (lower panel) of 2-phenyllactic acid at -1.8 V vs. Ag/AgI for different catalysts. (d) The stability test of Ag-CeO2 NWs at -1.8 V vs. Ag/AgI.

Fig. 5. The proposed two formation mechanisms of electrocarboxylation between acetophenone and CO2 on the Ag-CeO2 NW catalyst.

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通过双活化策略在Ag-CeO₂电催化剂上用苯乙酮高效固定CO₂

Efficient CO₂ fixation with acetophenone on Ag-CeO₂ electrocatalyst by a double activation strategy

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