Cu纳米针上电场促进C-C耦合增强CO2电还原生成C2产物

doi:10.1016/S1872-2067(21)63866-4

催化学报 ›› 2022, Vol. 43 ›› Issue (2): 519-525.DOI: 10.1016/S1872-2067(21)63866-4

Cu纳米针上电场促进C-C耦合增强CO₂电还原生成C₂产物

李黄经纬^a, 周惠敏^a, 周亚姣^a, 胡俊华^b, MasahiroMiyauchi^c, 傅俊伟^a^,^#(), 刘敏^a^,^*()

^a中南大学物理与电子学院, 湖南省化学能源重点实验室, 粉末冶金国家重点实验室, 湖南长沙 410083, 中国
^b郑州大学材料科学与工程学院, 河南郑州 450002, 中国
^c东京工业大学材料与化工技术学院, 材料与科学工程系, 东京, 日本

收稿日期:2021-05-07 接受日期:2021-05-07 出版日期:2022-02-18 发布日期:2021-06-28
通讯作者: 傅俊伟,刘敏
基金资助:
国家自然科学基金(21872174);国家自然科学基金(22002189);国家自然科学基金(U1932148);国家科技部重点研发国际间合作项目(2017YFE0127800);国家科技部重点研发国际间合作项目(2018YFE0203402);湖南省重点领域研发计划(2020WK2002);湖南省自然科学基金(2020JJ2041);湖南省自然科学基金(2020JJ5691);湖南省科技计划项目(2017XK20262);湖南省科技计划项目(2017TP1001);深圳科技创新项目(JCYJ20180307151313532);中南大学中央高校基本科研业务费专项资金

Electric-field promoted C-C coupling over Cu nanoneedles for CO₂ electroreduction to C₂ products

HuangJingWei Li^a, Huimin Zhou^a, Yajiao Zhou^a, Junhua Hu^b, Masahiro Miyauchi^c, Junwei Fu^a^,^#(), Min Liu^a^,^*()

^aHunan Provincial Key Laboratory of Chemical Power Sources, State Key Laboratory of Powder Metallurgy, School of Physics and Electronics, Central South University, Changsha 410083, Hunan, China
^bSchool of Materials Science and Engineering, Zhengzhou University, Zhengzhou 450002, Henan, China
^cDepartment of Materials Science and Engineering, School of Materials and Chemical Technology, Tokyo Institute of Technology, Tokyo 152-8552, Japan

Received:2021-05-07 Accepted:2021-05-07 Online:2022-02-18 Published:2021-06-28
Contact: Junwei Fu, Min Liu
Supported by:
This work was supported by the National Natural Science Foundation of China(21872174);This work was supported by the National Natural Science Foundation of China(22002189);This work was supported by the National Natural Science Foundation of China(U1932148);International Science and Technology Cooperation Program(2017YFE0127800);International Science and Technology Cooperation Program(2018YFE0203402);Hunan Province Key Field R&D Program(2020WK2002);Hunan Provincial Natural Science Foundation of China(2020JJ2041);Hunan Provincial Natural Science Foundation of China(2020JJ5691);the Hunan Provincial Science and Technology Plan Project(2017XK20262);the Hunan Provincial Science and Technology Plan Project(2017TP1001);Shenzhen Science and Technology Innovation Project(JCYJ20180307151313532);the Fundamental Research Funds for the Central Universities of Central South University

摘要/Abstract

摘要：

电催化CO₂减排技术利用电能将过量的CO₂转化为有附加值的化学品, 是解决能源危机、实现碳中和的有效途径之一. 电催化CO₂还原反应(CO₂RR)中的多碳产物(C₂), 如乙烯和乙醇, 因其比C₁产物具有更高的能量密度和更广泛的应用而受到较大关注. 目前为止, Cu基催化剂被认为是获得C₂产物的独特材料. 研究者在提高Cu基催化剂C₂产物的活性和选择性方面做了大量的工作, 如催化剂形貌工程、活性位点设计和中间吸附性能调控等. 许多理论和实验研究已经证明, Cu基催化剂上的C-C偶联过程是C₂产物生成的速率决定步骤. 优化C-C偶联过程的能垒是提高C₂产物活性和选择性的重要而直接的策略. CO₂RR在Cu上是由CO₂还原吸附CO(*CO)并二聚生成C₂产物引起的. C-C偶联过程与*CO的吸附性能密切相关. 众所周知, CO是一种典型的极性分子, 因此其在催化剂表面的吸附性能可能会受到活性位点周围的局部电场的影响. 构建合适的局部电场是调节CO吸附性能和C-C偶联过程的潜在手段之一. 前期工作(Nature, 2016, 537, 382-386)证明了高曲率金纳米针可以在尖端产生高的局部电场. 高局域电场诱导K ⁺聚集, 使活性位点周围CO₂浓度升高, 大大促进了Au纳米针上的CO生成.
基于Au纳米针的局域电场促进了CO₂RR的CO生成. 本文利用Cu纳米针促进并优化C-C偶联反应来提高C₂产物活性和选择性. 结果表明, 局部电场可以促进C-C偶联过程, 进而增强CO₂电还原生成C₂产物. 有限元模拟结果表明, 高曲率铜纳米针处存在较强的局部电场; 密度泛函理论计算结果表明, 强电场能促进C-C耦合过程. 在此基础上, 制备了一系列不同曲率的Cu催化剂, 其中, Cu纳米针(Cu NNs)的曲率最高, Cu纳米棒(Cu NRs)和Cu纳米颗粒(Cu NPs)曲率次之. 实验测得Cu NNs上吸附的K ⁺浓度最高, 证明了纳米针上的局部电场最强. 同时, CO吸附传感器测试表明, Cu NNs对CO的吸附能力最强, 原位傅里叶变换红外光谱显示, Cu NNs的*COCO和*CO信号最强. 由此可见, 高曲率铜纳米针可以诱导高局部电场, 从而促进C-C耦合过程. 催化性能测试结果表明, 在低电位(-0.6 V vs. RHE)下, Cu NNs对CO₂RR的生成C₂产物的法拉第效率值为44%, 约为Cu NPs的2.2倍. 综上, 本文为CO₂RR过程中提高多碳产物提供了新的思路.

关键词: 电场效应, C-C偶联, 铜纳米针, C₂产物, 二氧化碳还原

Abstract:

Cu-based catalysts are the most promising candidates for electrochemical CO₂ reduction (CO₂RR) to multi-carbon (C₂) products. Optimizing the C-C coupling process, the rate-determining step for C₂ product generation, is an important strategy to improve the production and selectivity of the C₂ products. In this study, we determined that the local electric field can promote the C-C coupling reaction and enhance CO₂ electroreduction to C₂ products. First, finite-element simulations indicated that the high curvature of the Cu nanoneedles results in a large local electric field on their tips. Density functional theory (DFT) calculations proved that a large electric field can promote C-C coupling. Motivated by this prediction, we prepared a series of Cu catalysts with different curvatures. The Cu nanoneedles (NNs) exhibited the largest number of curvatures, followed by the Cu nanorods (NRs), and Cu nanoparticles (NPs). The Cu NNs contained the highest concentration of adsorbed K ⁺, which resulted in the highest local electric field on the needles. CO adsorption sensor tests indicated that the Cu NNs exhibited the strongest CO adsorption ability, and in-situ Fourier-transform infrared spectroscopy (FTIR) showed the strongest *COCO and *CO signals for the Cu NNs. These experimental results demonstrate that high-curvature nanoneedles can induce a large local electric field, thus promoting C-C coupling. As a result, the Cu NNs show a maximum FE_C2 of 44% for CO₂RR at a low potential (-0.6 V vs. RHE), which is approximately 2.2 times that of the Cu NPs. This work provides an effective strategy for enhancing the production of multi-carbon products during CO₂RR.

Key words: Electric-field effect, C-C coupling, Cu nanoneedle, C₂ products, CO₂ electroreduction

李黄经纬, 周惠敏, 周亚姣, 胡俊华, MasahiroMiyauchi, 傅俊伟, 刘敏. Cu纳米针上电场促进C-C耦合增强CO₂电还原生成C₂产物[J]. 催化学报, 2022, 43(2): 519-525.

HuangJingWei Li, Huimin Zhou, Yajiao Zhou, Junhua Hu, Masahiro Miyauchi, Junwei Fu, Min Liu. Electric-field promoted C-C coupling over Cu nanoneedles for CO₂ electroreduction to C₂ products[J]. Chinese Journal of Catalysis, 2022, 43(2): 519-525.

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图/表 5

Fig. 1(a) shows the distribution of the electric field intensity on the surface of the Cu catalysts exhibiting different curvatures. The radii at the tips of the NNs, NRs, and NPs were set to 10, 50, and 150 nm, respectively. The corresponding electric field intensities (shown in Fig. 1(b)) at the tips of the Cu NNs, Cu NRs, and Cu NPs are 8.12, 5.36, and 2.01 kV/m, respectively. These results indicate that the Cu NNs, which are more curved, exhibit the strongest electric field.

Fig. 1. (a) Simulated electric field distribution on the surfaces of the Cu NNs, Cu NRs, and Cu NPs with different curvatures; (b) Electric field intensity at the tips of the Cu NNs, Cu NRs, and Cu NPs; (c) Simulated K+ concentrations at the tips of the Cu NNs, Cu NRs, and Cu NPs; (d) DFT calculated reaction barriers of the C-C coupling reaction on the surface of Cu(100) under different electric field intensities; (e) Schematic diagram of the C-C coupling reaction on the surface of Cu(100) with and without an applied electric field.

Fig. 2. (a) Schematic of the preparation process for the Cu-based catalysts with different curvatures; (b) XRD patterns of the Cu NPs, Cu NRs, and Cu NNs after electrochemical reduction at 10 mA cm-2 for 1000 s in a CO2-saturated solution; (c-e) Corresponding SEM images of the Cu NPs, Cu NRs, and Cu NNs; (f-h) Enlarged SEM images of the Cu NPs, Cu NRs, and Cu NNs.

Fig. 3. (a) The measured K+ concentration in the Cu NPs, Cu NRs, and Cu NNs; (b) The current density differences of the Cu NPs, Cu NRs, and Cu NNs under CO atmosphere and under vacuum at 0, 0.1, and 0.2 V; (c) The in-situ FTIR spectra of the Cu NNs, Cu NRs, and Cu NPs between 1540 and 1610 cm-1.

Fig. 4. (a) Product distribution of the Cu NNs, Cu NRs, and Cu NPs at -0.6 V vs. RHE; FEC2 (b) and current density (c) of the Cu NNs, Cu NRs, and Cu NPs at different potentials; (d) Stability test of the Cu NNs, Cu NRs, and Cu NPs at -0.6 V vs. RHE.

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Cu纳米针上电场促进C-C耦合增强CO₂电还原生成C₂产物

Electric-field promoted C-C coupling over Cu nanoneedles for CO₂ electroreduction to C₂ products

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