Sun Zengsen, Wu Xinhao, Guan Daqin, Chen Xiaoyi, Dai Jie, Gu Yuxing, She Sixuan, Zhou Wei, Shao Zongping
State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University, Nanjing 211800, P. R. China.
School of Mechanical and Power Engineering, Nanjing Tech University, Nanjing 211800, P. R. China.
ACS Appl Mater Interfaces. 2021 Dec 22;13(50):59993-60001. doi: 10.1021/acsami.1c19529. Epub 2021 Dec 10.
Electrochemical CO reduction (ECR) technology is promising to produce value-added chemicals and alleviate the climate deterioration. Interface engineering is demonstrated to improve the ECR performance for metal and oxide composite catalysts. However, the approach to form a substantial interface is still limited. In this work, we report a facile one-pot coprecipitation method to synthetize novel silver and silver-doped ceria (Ag/CeO) nanocomposites. This catalyst provides a rich 3D interface and high Ce concentration (33.6%), both of which are beneficial for ECR to CO. As a result, Ag/CeO exhibits a 99% faradaic efficiency and 10.5 A g mass activity to convert CO into CO at an overpotential of 0.83 V. The strong interfacial interaction between Ag and CeO may enable the presence of surface Ce and guarantee the improved durability during the electrolysis. We also develop numerical simulation to understand the local pH effect on the ECR performance and propose that the superior ECR performance of Ag/CeO is mainly due to the accelerated CO formation rate rather than the suppressed hydrogen evolution reaction.
电化学CO还原（ECR）技术有望生产增值化学品并缓解气候恶化。界面工程已被证明可改善金属和氧化物复合催化剂的ECR性能。然而，形成大量界面的方法仍然有限。在这项工作中，我们报告了一种简便的一锅共沉淀法来合成新型银和银掺杂二氧化铈（Ag/CeO）纳米复合材料。这种催化剂提供了丰富的三维界面和高Ce浓度（33.6%），这两者都有利于将ECR转化为CO。结果，Ag/CeO在0.83 V的过电位下将CO转化为CO时表现出99%的法拉第效率和10.5 A g的质量活性。Ag和CeO之间强烈的界面相互作用可能使表面Ce存在，并保证电解过程中耐久性的提高。我们还开展了数值模拟以了解局部pH对ECR性能的影响，并提出Ag/CeO优异的ECR性能主要归因于加速的CO生成速率而非抑制的析氢反应。
