铜泡沫上铋纳米片的形成与纳米气泡技术相结合,增强二氧化碳的电催化还原能力

IF 10.7 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Kai Wu, Pengwei Yang, Shuaijun Fan, Yifan Wu, Jingxiang Ma, Lijuan Yang, Hongtao Zhu, Xiaoying Ma, Heli Gao, Wentong Chen, Jun Jia, Shuangchen Ma
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引用次数: 0

摘要

回收利用工业排放的二氧化碳是一项紧迫的环保任务。用电化学方法将二氧化碳还原成有价值的化学产品是一种极具吸引力的方法。然而,由于二氧化碳分子固有的高化学稳定性以及二氧化碳还原反应(CO2RR)中涉及的多个电子和质子转移步骤的复杂顺序,目前的电催化系统普遍面临着二氧化碳转化率和能量利用效率低、电流密度有限以及电极寿命短等挑战。在此,我们采用原位化学蚀刻、热氧化和电化学还原的简单三步法,在泡沫铜上构建出具有丰富晶格位错的纳米铋片(Bi NSs),并引入纳米气泡技术来增强 CO2RR 过程。在带有流动电解质的 H 型电池中,我们的 Bi NSs/CF 电极在相对于 RHE(可逆氢电极)-1.08 V 的低应用电位下实现了 95.36% 的显著甲酸法拉第效率 (FEFormate),以及约 38 mA cm-2 的显著甲酸部分电流密度 (JFormate) 和约 60% 的能量效率。即使在更宽的操作窗口(-0.78 至 -1.18 V)内,甲酸盐部分电流密度仍保持在较高水平(91%)。重要的是,纳米气泡技术的应用使二氧化碳转化率提高了近五倍。进一步的密度泛函理论计算证实,在 Bi NSs/CF 表面具有晶格位错的 Bi NSs 能有效稳定 *OCHO 中间体,从而实现 CO2RR 的高活性和高选择性。这项工作凸显了纳米气泡技术、尺寸依赖催化和晶体缺陷工程策略在电催化领域的重要作用,阐明了所开发催化剂在电化学 CO2 还原过程中的活性来源,为 CO2RR 及其他领域高性能电催化系统的设计和开发提供了宝贵的启示。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Formation of Bismuth Nanosheets on Copper Foam Coupled with Nanobubble Technology for Enhanced Electrocatalytic CO2 Reduction
The recycling of industrially emitted CO2 is an urgent environmental task. Electrochemical reduction of CO2 into valuable chemical products presents an attractive approach. However, due to the inherent high chemical stability of CO2 molecules and the complex sequence of multiple electron and proton transfer steps involved in the CO2 reduction reaction (CO2RR), current electrocatalytic systems commonly face challenges such as low CO2 conversion rates and energy utilization efficiency, limited current density, and short electrode lifespan. Herein, we adopt a simple three-step process involving in situ chemical etching, thermal oxidation, and electrochemical reduction to construct bismuth nanosheets (Bi NSs) with abundant lattice dislocations on copper foam, and introduce nanobubble technology to enhance the CO2RR process. In an H-type cell with flowing electrolyte, our Bi NSs/CF electrode achieved a remarkable formate Faradaic efficiency (FEFormate) of 95.36% at a low applied potential of -1.08 V vs. RHE (reversible hydrogen electrode), along with a significant formate partial current density (JFormate) of ~38 mA cm-2 and an energy efficiency of ~60%. Even within a wider operating window (-0.78 to -1.18 V), the FEFormate remained at a high level (>91%). Importantly, the application of nanobubble technology made the CO2 conversion rate increase nearly fivefold. Further density functional theory calculations confirmed that the Bi NSs with lattice dislocations on the Bi NSs/CF surface can effectively stabilize the *OCHO intermediate, thereby achieving high activity and selectivity for CO2RR. This work highlights the significant roles of nanobubble technology, size-dependent catalysis, and crystal defect engineering strategies in the field of electrocatalysis, elucidating the activity sources of the developed catalyst in the electrochemical CO2 reduction process, and providing valuable insights for the design and development of high-performance electrocatalytic systems for CO2RR and other fields.
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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