Syngas production from electrocatalytic CO2 reduction with high energetic efficiency and current density
Syngas production from electrocatalytic CO2 reduction with high energetic efficiency and current density
复制标题
通过电催化二氧化碳还原生产合成气，具有高能量效率和电流密度
DOI：
10.1039/c9ta01932d
复制
发表时间：
2019-04-07
影响因子：
11.9
通讯作者：
Qiao, Shi-Zhang
中科院分区：
文献类型：
--
作者：
Chen, Ping;Jiao, Yan;Qiao, Shi-Zhang
将CO2直接转化为具有可控组成的合成气仍然是生产可再生燃料的强烈兴趣。大电流密度和高电池电压效率对于电化学CO2还原反应（CRR）的实用性至关重要，而催化剂的设计是一个巨大的挑战。在这里，我们报告氧化物衍生的铜纳米线与丰富的，高度分散的两相氧化铜异质结构的合成气产生。实现了指定的H-2/CO比1、2和3，具有超高的CRR法拉第（90%）和能量（50%）效率。密度泛函理论计算表明，电催化剂中的错配位错位打破了CRR中间体吸附能与 *COOH的强吸附之间的内在标度关系，从而促进了催化剂对CRR的优异活性。在商业太阳能电池（工作电压为2.2V）的直接阳光下驱动，独立式电催化剂可以使用CO2作为原料稳定地产生所需组成的合成气。
The direct conversion of CO2 to syngas with controllable composition remains an intense interest for the production of renewable fuels. Large current density and high cell voltage efficiency are critical from a practical viewpoint for electrochemical CO2 reduction reaction (CRR), while the design of catalysts is a great challenge. Here, we report oxide-derived Cu nanowires with abundant, highly dispersed two-phase CuO heterostructures for syngas generation. The specified H-2/CO ratios of 1, 2 and 3, with extra high CRR faradic (90%) and energetic (50%) efficiencies, were achieved. Density functional theory calculations reveal that the misfit dislocation sites in the electrocatalyst break the inherent scaling relationship of CRR intermediates' adsorption energies with an extraordinarily strong adsorption of *COOH and consequently promote excellent activity of the catalyst toward CRR. Driven by a commercial solar cell (working voltage of 2.2 V) under direct sunlight, the freestanding electrocatalyst can steadily generate syngas of the desired composition using CO2 as a feedstock.