Nitrogen, Sulfur Co-Doped Hierarchically Porous Carbon as a Metal-Free Electrocatalyst for Oxygen Reduction and Carbon Dioxide Reduction Reaction
Nitrogen, Sulfur Co-Doped Hierarchically Porous Carbon as a Metal-Free Electrocatalyst for Oxygen Reduction and Carbon Dioxide Reduction Reaction
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氮、硫共掺杂多级孔碳作为氧还原和二氧化碳还原反应的无金属电催化剂
DOI：
10.1021/acsami.0c06506
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发表时间：
2020-10-07
影响因子：
9.5
通讯作者：
Liu, Dong
中科院分区：
文献类型：
--
作者：
Li, Ruru;Liu, Feng;Liu, Dong
高成本和低效率的电催化剂阻碍了燃料电池中的氧还原反应（ORR）和用于生产燃料和增值化学品的CO2还原反应（CO2RR）。在这里，低成本的无金属的N，S共掺杂的分级多孔碳（NSHPC）的有效的ORR和CO2RR的电催化剂的报告。以SiO2为硬模板剂，通过热解氨基葡萄糖盐酸盐和硫氰尿酸前体制备了NSHPC。N，S共掺杂有效地提高了催化活性和选择性，并且分级多孔结构在很大程度上将丰富的活性位点暴露给反应物种并促进电解质传输，从而导致NSHPC的催化活性显著提高。所得NSHPC在酸性和碱性电解质中都表现出优异的对ORR的电催化活性，并且还显示出在质子交换膜燃料电池（PEMFC）中的应用。更重要的是，NSHPC能够在水性电解质中以87.8%的最大法拉第效率（FE）将CO2还原为CO。这项工作为开发用于生产电力，燃料和增值化学品的多功能电催化剂提供了新的见解。
High-cost and low-efficiency electrocatalysts have hindered oxygen reduction reaction (ORR) in fuel cells and CO2 reduction reaction (CO2RR) for producing fuels and value-added chemicals. Here, a low-cost metal-free electrocatalyst of a N, S co-doped hierarchically porous carbon (NSHPC) for efficient ORR and CO2RR is reported. The NSHPC is prepared by pyrolysis of glucosamine hydrochloride and thiocyanuric acid precursors using SiO2 as hard templates. The N, S co-doping effectively enhances catalytic activity and selectivity, and the hierarchically porous structure largely exposes abundant active sites to reaction species and facilitates electrolyte transport, thereby leading to significantly increased catalytic activities for the NSHPC. The resultant NSHPC exhibits excellent electrocatalytic activities toward ORR in both acidic and alkaline electrolytes and also shows application in proton exchange membrane fuel cells (PEMFCs). More importantly, the NSHPC enables CO2 reduction to CO with 87.8% maximum Faraday efficiency (FE) in aqueous electrolytes. This work offers a novel insight into the development of multifunctional electrocatalysts for producing electricity, fuels, and value-added chemicals.