原位构筑动态Cu/Ce(OH)x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨

doi:10.1016/S1872-2067(23)64506-1

催化学报 ›› 2023, Vol. 52: 196-206.DOI: 10.1016/S1872-2067(23)64506-1

原位构筑动态Cu/Ce(OH)_x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨

刘勇^a^,^b, 赵晓丽^a^,^c, 隆昶^d, 王晓艳^a, 邓邦为^a, 李康璐^e^,^f, 孙艳娟^a^,^c, 董帆^a^,^e^,^*()

^a电子科技大学长三角研究院(湖州), 浙江湖州313000
^b成都信息工程大学光电工程学院, 四川成都610225
^c电子科技大学资源与环境学院, 四川成都611731
^d电子科技大学基础与前沿研究院, 分子电化学实验室, 四川成都610054
^e电子科技大学基础与前沿研究院, 碳中和环境与能源技术研究中心, 四川成都611731
^f四川大学建筑与环境学院, 四川成都610065

收稿日期:2023-05-03 接受日期:2023-08-21 出版日期:2023-09-18 发布日期:2023-09-25
通讯作者: *电子信箱: dfctbu@126.com,dongfan@uestc.edu.cn (董帆).
基金资助:
国家重点研发计划(2020YFA0710000);国家自然科学基金(22225606);国家自然科学基金(22176029);四川省自然科学杰出学者基金(2021JDJQ0006)

In situ constructed dynamic Cu/Ce(OH)_x interface for nitrate reduction to ammonia with high activity, selectivity and stability

Yong Liu^a^,^b, Xiaoli Zhao^a^,^c, Chang Long^d, Xiaoyan Wang^a, Bangwei Deng^a, Kanglu Li^e^,^f, Yanjuan Sun^a^,^c, Fan Dong^a^,^e^,^*()

^aYangtze Delta Region Institute (Huzhou), University of Electronic Science and Technology of China, Huzhou 313000, Zhejiang, China
^bCollege of Optoelectronic Engineering, Chengdu University of Information Technology, Chengdu 610225, Sichuan, China
^cSchool of Resources and Environment, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
^dMolecular Electrochemistry Laboratory, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 610054, Sichuan, China
^eResearch Center for Carbon-Neutral Environmental & Energy Technology, Institute of Fundamental and Frontier Sciences, University of Electronic Science and Technology of China, Chengdu 611731, Sichuan, China
^fCollege of Architecture and Environment, Sichuan University, Chengdu 610065, Sichuan, China

Received:2023-05-03 Accepted:2023-08-21 Online:2023-09-18 Published:2023-09-25
Contact: *E-mail: dfctbu@126.com,dongfan@uestc.edu.cn (F. Dong).
Supported by:
National Key R&D Program of China(2020YFA0710000);National Natural Science Foundation of China(22225606);National Natural Science Foundation of China(22176029);Sichuan Natural Science Foundation for Distinguished Scholars(2021JDJQ0006)

摘要/Abstract

摘要：

电催化硝酸根还原反应(NO₃^‒RR)使用电子作为绿色还原剂, 为去除和利用水中硝酸盐提供了一种有前景的技术. 其中, 铜基材料在碱性溶液(如1 mol L^‒1 KOH)中显示出较高的NO₃^‒RR催化活性, 但在中性条件下催化剂的性能不高. 目前, 在中性体系中同时实现高活性、高选择性和高法拉第效率的氨合成是一个巨大的挑战. 以往研究主要通过掺杂、合金化、调节晶面和引入缺陷等办法来提高NO₃^‒RR的性能. 此外, 构筑异质结构界面可以调节催化剂的几何结构、电荷分布和配位环境, 也是优化催化性能的一种有效策略. 通过异质结构界面效应可以提供更多的催化活性位点, 打破单组分催化剂的活性线性关系, 进而提升NO₃^‒RR性能. 已有的研究中多采用直接化学合成法构筑铜基异质结催化剂, 但在NO₃^‒RR条件下原位制备异质结催化剂的文献报道较少, 且已有的少数在NO₃^‒RR条件下原位制备铜基异质结构的报道, 由于界面性质不利、活性位点密度低, 其催化NO₃^‒RR的性能难以令人满意. 因此, 有必要采取有效的策略来原位构筑具有可调界面结构和丰富活性位点的铜基异质结构.

本文提出了一种原位动态重构策略, 通过构筑具有丰富界面活性位点的Cu/Ce(OH)_x催化剂以提高NO₃^‒RR性能. 在KCl溶液中将Ce(OH)_x电沉积到泡沫铜上, 生成Cu₂Cl(OH)₃并与Ce(OH)_x一起沉积形成Cu₂Cl(OH)₃/Ce(OH)_x异质结构. 在NO₃^‒RR过程中, Cu₂Cl(OH)₃/Ce(OH)_x经历动态重构, 原位形成了Cu/Ce(OH)_x催化剂. 原位活化后, NO₃^‒RR性能显著增强, 随后达到稳定状态. 催化剂展现出较好的催化性能, NO₃^‒转化率为100.0%, NH₃选择性为97.8%, NH₃法拉第效率为99.2%, 并表现出长期稳定性, 是中性介质中较先进的催化剂之一. 采用X射线衍射(XRD)、扫描电镜(SEM)、高分辨透射电镜(HRTEM)、选区电子衍射(SAED)、X射线光电子能谱(XPS)及原位拉曼光谱表征了Cu₂Cl(OH)₃/Ce(OH)_x预催化剂的原位重构过程. XRD结果表明, Cu₂Cl(OH)₃/Ce(OH)_x预催化剂在第一次NO₃^‒RR测试后还原形成了Cu/Ce(OH)_x. SEM结果表明, Cu₂Cl(OH)₃颗粒在第一次NO₃^‒RR循环后开始形成裂纹, 第二次NO₃^‒RR后碎裂成几十至100 nm的颗粒, 其上存在大量Ce(OH)_x纳米粒子. HRTEM和SAED结果证实了上述结构变化. XPS结果表明, 铜在原位重构过程中逐渐从高价态还原到低价态. 原位拉曼光谱进一步确认Cu₂Cl(OH)₃还原为Cu₂O再到Cu的动态转变过程. 原位和非原位表征结果一致表明, Cu₂Cl(OH)₃/Ce(OH)_x异质结构经历了动态还原和纳米化过程, 原位构筑了具有丰富活性位点的Cu/Ce(OH)_x界面. 采用在线微分电化学质谱(DEMS)和密度泛函理论(DFT)研究了NO₃^‒RR性能增强机理. DEMS结果表明, Cu/Ce(OH)_x上存在NO, HNO/NOH和NH₂OH中间体. DFT结果表明, Cu/Ce(OH)_x界面位点具有以下作用: (1) 促进硝酸根的吸附和活化; (2) 降低了电位限制步骤(NO*→HNO*)的反应能垒; (3) 通过增强氢吸附强度, 抑制了析氢副反应的发生. 此外, 原位纳米化形成的丰富界面活性位点也促进了NO₃^‒RR活性的提升.

综上, 本文提出了一种原位构筑动态界面活性位点的策略, 从而增强电催化性能, 以实现高价值化学品的可持续合成. 未来可改变前驱体种类将该方法拓展至其他催化剂体系, 探索其在多种电催化反应中的应用.

关键词: 金属/氢氧化物界面, 原位构筑, 电催化硝酸根还原, 氨合成, 选择性

Abstract:

Electrocatalytic nitrate reduction (NO₃^‒RR) offers a promising technique for the removal and utilization of nitrate in water. However, the performance of current catalysts is still limited mainly due to the unfavorable interface that largely determines the reaction efficiency and selectivity. Here we present an in situ dynamic reconstruction strategy to enhance the NO₃^‒RR by constructing Cu/Ce(OH)_x catalyst with abundant interfacial active sites. The Cu/Ce(OH)_x catalyst was in situ formed through dynamic reconstruction of Cu₂Cl(OH)₃/Ce(OH)_x heterostructure during electrochemical NO₃^‒RR process. The catalyst exhibits high performance with NO₃^‒ conversion of 100.0%, NH₃ selectivity of 97.8%, NH₃ Faradaic efficiency of 99.2% and long stability, which is among the state-of-the-art catalysts in neutral media. Both experimental and theoretical results demonstrate that the Cu and Ce sites at the interface can operate cooperatively to promote the adsorption and activation of NO₃^‒, and lower the formation energy of key intermediate *HNO. Meanwhile, the hydrogen evolution reaction is also greatly suppressed due to the high H* binding strength at the interface. The strategy can be extended to other catalytic systems and opens a new avenue for the design of efficient electrocatalysts.

Key words: Metal/hydroxide interface, In situ construction, Electrocatalytic nitrate reduction, Ammonia synthesis, Selectivity

刘勇, 赵晓丽, 隆昶, 王晓艳, 邓邦为, 李康璐, 孙艳娟, 董帆. 原位构筑动态Cu/Ce(OH)_x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨[J]. 催化学报, 2023, 52: 196-206.

Yong Liu, Xiaoli Zhao, Chang Long, Xiaoyan Wang, Bangwei Deng, Kanglu Li, Yanjuan Sun, Fan Dong. In situ constructed dynamic Cu/Ce(OH)_x interface for nitrate reduction to ammonia with high activity, selectivity and stability[J]. Chinese Journal of Catalysis, 2023, 52: 196-206.

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https://www.cjcatal.com/CN/Y2023/V52/I9/196

图/表 5

Fig. 1. NO3-RR performance of Cu/Ce(OH)x-30 catalyst. (a) LSV curves of Cu/Ce(OH)x-30 with and without NO3-. NO3- conversion (b) and NH3 selectivity and Faradaic efficiency (c) in twelve consecutive cycling tests at ?0.6 V vs. RHE. (d) Comparison of the NO3-RR performance in 0.1 mol L?1 K2SO4 and 0.1 mol L?1 PBS.

Fig. 2. NO3-RR performance of Cu/Ce(OH)x at different conditions. NH3 and NO2- selectivity (a), NH3 Faradaic efficiency and yield rate (b) over Cu/Ce(OH)x-30 at different applied potentials. (c) NO3?RR performance of Cu/Ce(OH)x-30 at different initial NO3- concentrations. (d) NH3 and NO2- selectivity over Cu/Ce(OH)x catalysts with different electrodeposition time at ?0.6 V vs. RHE.

Fig. 3. SEM and TEM images of Cu/Ce(OH)x. SEM images of Cu/Ce(OH)x before (a) and after one (b) and two (c) electrocatalytic cycles. TEM images of Cu/Ce(OH)x before (d?f) and after (g,h) two electrocatalytic cycles. Insets in e and f are the corresponding SAED patterns. HAADF-STEM (i,j) and elemental mapping images (k?m) after two electrocatalytic cycles.

Fig. 4. Cu 2p (a) and Ce 3d (b) XPS spectra of Cu/Ce(OH)x before and after different electrocatalytic cycles. (c) In situ Raman spectra collected during NO3-RR at ?0.6 V vs. RHE.

Fig. 5. Charge density difference and adsorption energy of NO3 on Cu(111)/Ce3O7H3 (a) and Cu(111) (b) surface. The yellow and cyan colors represent charge accumulation and depletion, respectively. The isosurface level is set to be 0.005 e ??3. Δq indicates number of electrons transferred from the catalysts to adsorbed NO3. On line DEMS measurements during NO3?RR over Cu/Ce(OH)x (c) and copper (d) foam. (e) Reaction free energy diagram on Cu(111) and Cu(111)/Ce3O7H3 surface. Ce, Cu, O, N, and H atoms are shown as beige, orange, red, blue and white spheres, respectively.

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原位构筑动态Cu/Ce(OH)_x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨

In situ constructed dynamic Cu/Ce(OH)_x interface for nitrate reduction to ammonia with high activity, selectivity and stability

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原位构筑动态Cu/Ce(OH)x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨

In situ constructed dynamic Cu/Ce(OH)x interface for nitrate reduction to ammonia with high activity, selectivity and stability

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原位构筑动态Cu/Ce(OH)_x界面用于高活性、高选择性和高稳定性硝酸盐还原合成氨

In situ constructed dynamic Cu/Ce(OH)_x interface for nitrate reduction to ammonia with high activity, selectivity and stability