碳层网络促进Sn/SnO2纳米颗粒选择性CO2还原

doi:10.13208/j.electrochem.210844

摘要/Abstract

摘要：

在各类CO₂还原电催化剂中,锡基材料获得了研究人员的广泛关注,但其总体催化性能仍然受催化剂电极的组成,形貌和结构的限制。在本研究中,我们利用Sn低熔点（m.p. 232^oC）的特性,在聚多巴胺碳化的同时实现Sn的熔化与再结晶,合成了由氮掺杂碳层网络分散的异质结构Sn/SnO₂纳米颗粒自支撑电极（Sn/SnO₂@NC）。氮掺杂碳层网络有利于电子的富集,可提高催化剂电极的导电性,防止超细纳米粒子的团聚,并保护其不在电解液中溶解。在CO₂饱和的0.5 mol·L^-1 NaHCO₃水溶液中,所制备Sn/SnO₂@NC电极与没有碳层网络包覆的电极相比,其CO₂还原催化性能得到了很大的提高。该Sn/SnO₂@NC电极在-0.9 V（vs. RHE）的电解电压下,电流密度为17 mA·cm^-2,甲酸盐产物的选择性为83%。通过偶联该CO₂还原催化电极与商品化RuO₂催化剂作为水氧化阳极,可实现持续的CO₂/H₂O电解。此外,以Sn/SnO₂@NC为阴极,Zn箔为阳极,我们还构建了可充放电的水系Zn-CO₂电池。该电池的输出开路电压为1.35 V,峰值功率密度为0.9 mW·cm^-2。本研究为高性能CO₂还原催化剂的设计提供了新的思路,同时可充放电Zn-CO₂电池的构建为绿色能源转换和存储系统提供了新的方案。

关键词: CO₂电催化还原, 碳层网络, Sn/SnO₂, 甲酸, Zn-CO₂电池

Abstract:

Tin (Sn)-based materials have emerged as promising electrocatalysts for selective reduction of CO₂ to formate, but their overall performances are still limited by electrode structures which govern the accessibility to active sites, the electron transfer kinetics, and the catalytic stability. In this study, the heterostructured Sn/SnO₂ nanoparticles dispersed by N-doped carbon layer networks (Sn/SnO₂@NC) were synthesized by a melt-recrystallization method taking the low melting point of Sn (m.p. 232^oC). The N-doped carbon layer networks derived from polydopamine could attract more electrons on the electrocatalyst, serve as conductive agents and protect the ultrafine nanoparticles from agglomeration and dissolution. The Sn/SnO₂@NC electrode exhibited the greatly enhanced performance for CO₂ reduction to formate in CO₂-saturated 0.5 mol·L^-1 aqueous NaHCO₃ solution, showing a selectivity of 83% at only -0.9 V vs. RHE with a sustained current density of 17 mA·cm^-2 for extended periods. By coupling the catalytic electrode with a commercially available RuO₂ catalyst as the anode, the long-term CO₂/H₂O splitting has been achieved. Furthermore, a rechargeable aqueous Zn-CO₂ battery with Sn/SnO₂@NC as the cathode and Zn foil as the anode was constructed. It could output electric energy with an open circuit voltage of 1.35 V and a peak power density of 0.9 mW·cm^-2.

Key words: CO₂ electrochemical reduction, carbon layer networks, Sn/SnO₂, formate, Zn-CO₂ batteries

滕雪, 牛艳丽, 巩帅奇, 刘璇, 陈作锋. 碳层网络促进Sn/SnO₂纳米颗粒选择性CO₂还原[J]. 电化学（中英文）, 2022, 28(2): 2108441.

Xue Teng, Yanli Niu, Shuaiqi Gong, Xuan Liu, Zuofeng Chen. Selective CO₂ Reduction to Formate on Heterostructured Sn/SnO₂ Nanoparticles Promoted by Carbon Layer Networks[J]. Journal of Electrochemistry, 2022, 28(2): 2108441.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.210844

https://electrochem.xmu.edu.cn/CN/Y2022/V28/I2/2108441

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碳层网络促进Sn/SnO₂纳米颗粒选择性CO₂还原

Selective CO₂ Reduction to Formate on Heterostructured Sn/SnO₂ Nanoparticles Promoted by Carbon Layer Networks

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