Nitrogen-doped tubular carbon foam electrodes for efficient electroreduction of CO2 to syngas with potential-independent CO/H2 ratios
Nitrogen-doped tubular carbon foam electrodes for efficient electroreduction of CO2 to syngas with potential-independent CO/H2 ratios
复制标题
氮掺杂管状碳泡沫电极可有效地将 CO2 电还原为合成气，且 CO/H-2 比率与电势无关
DOI：
10.1039/c9ta05904k
复制
发表时间：
2019-08-28
影响因子：
11.9
通讯作者：
Qiu, Jieshan
中科院分区：
文献类型：
--
作者：
Li, Hongqiang;Xiao, Nan;Qiu, Jieshan
二氧化碳的电化学还原是生产合成气的一种很有前途的策略，合成气是生产各种工业化学品的重要原料。然而，由于有限的传质和低效的催化界面，实现稳定的CO/H-2电合成仍然是一个巨大的挑战。本论文设计了一系列氮气掺杂管状泡沫碳电极，作为气体扩散器和自负载电催化剂。由于二氧化碳的直接输送、强制对流和可调节的活性中心数量，单片管状电极能够在较宽的电势范围内(-0.5V到-1.3V对RHE)通过CO2还原有效地电合成CO/H-2比(1：3到2：1)可调的合成气。实验和模拟研究表明，新型管状泡沫炭结构显著增强了传质性能，提供了高效的三相催化界面，在高过电位区产生了相对稳定的合成气。
Electrochemical reduction of CO2 is a promising strategy to produce syngas, which is an essential feedstock for production of different industrial chemicals. However, it remains a great challenge to realize stable electrosynthesis of syngas with potential-independent CO/H-2 ratios due to the limited mass transport and inefficient catalytic interface. Herein, a series of nitrogen-doped tubular carbon foam electrodes were designed and used as both gas diffusers and self-supported electrocatalysts. Owing to the direct delivery of CO2, forced convection flow and tunable number of active sites, the monolithic tubular electrodes enable efficient electrosynthesis of syngas with tuned CO/H-2 ratios (1: 3 to 2 :1) by CO2 reduction in a wide potential range (-0.5 V to-1.3 V vs. RHE). Experimental and simulation studies reveal that the novel tubular carbon foam configuration significantly enhances the mass transport and provides an efficient triple-phase catalytic interface, resulting in relatively stable syngas production in the high-overpotential region.