Lu Song, Zhang Yang, Mady Mohamed F, Egwu Eleri Obinna, Mekonnen Tucho Wakshum, Mazur Michal, Li Ang, Lou Fengliu, Gu Minfen, Yu Zhixin
Department of Energy and Petroleum Engineering, University of Stavanger, 4036, Stavanger, Norway.
Beyonder AS, Kanalsletta 2, 4033, Stavanger, Norway.
ChemSusChem. 2022 Oct 10;15(19):e202200870. doi: 10.1002/cssc.202200870. Epub 2022 Sep 1.
Developing highly efficient electrocatalysts for electrochemical CO reduction (ECR) to value-added products is important for CO conversion and utilization technologies. In this work, a sulfur-doped Ni-N-C catalyst is fabricated through a facile ion-adsorption and pyrolysis treatment. The resulting Ni-NS-C catalyst exhibits higher activity in ECR to CO than S-free Ni-N-C, yielding a current density of 20.5 mA cm under -0.80 V versus a reversible hydrogen electrode (vs. RHE) and a maximum CO faradaic efficiency of nearly 100 %. It also displays excellent stability with negligible activity decay after electrocatalysis for 19 h. A combination of experimental investigations and DFT calculations demonstrates that the high activity and selectivity of ECR to CO is due to a synergistic effect of the S and Ni-N moieties. This work provides insights for the design and synthesis of nonmetal atom-decorated M-N-C-based ECR electrocatalysts.
开发用于电化学CO还原（ECR）以制备增值产品的高效电催化剂对于CO转化和利用技术至关重要。在这项工作中，通过简便的离子吸附和热解处理制备了硫掺杂的Ni-N-C催化剂。所得的Ni-NS-C催化剂在ECR制CO反应中表现出比无硫Ni-N-C更高的活性，在相对于可逆氢电极（vs. RHE）为-0.80 V的条件下，电流密度达到20.5 mA cm，CO法拉第效率最高接近100%。它还表现出优异的稳定性，在19小时的电催化后活性衰减可忽略不计。实验研究和DFT计算相结合表明，ECR制CO的高活性和选择性归因于S和Ni-N部分的协同作用。这项工作为设计和合成非金属原子修饰的M-N-C基ECR电催化剂提供了见解。
