State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Institute of High Energy Physics, The Chinese Academy of Sciences, Beijing, 100049, P. R. China.
Small. 2023 May;19(21):e2300581. doi: 10.1002/smll.202300581. Epub 2023 Feb 23.
Electrocatalytic reduction of CO to high-value-added chemicals provides a feasible path for global carbon balance. Herein, the fabrication of Ni @Ni -NG (x,y = 1, 2, 3; NG = nitrogen-doped graphite) is reported, in which Ni single atom sites (Ni ) and Ni nanoparticles (Ni ) coexist. These Ni @Ni -NG presented a volcano-like trend for maximum CO Faradaic efficiency (FE ) with the highest point at Ni @Ni -NG in CO RR. Ni @Ni -NG exhibited ≈98% of maximum FE and a large current density of -264 mA cm at -0.98 V (vs. RHE) in the flow cell. In situ experiment and density functional theory (DFT) calculations confirmed that the proper content of Ni and Ni balanced kinetic between proton-feeding and CO hydrogenation. The Ni in Ni @Ni -NG promoted the formation of H* and reduced the energy barrier of *CO hydrogenation to *COOH, and CO desorption can be efficiently facilitated by Ni sites, thereby resulting in enhanced CO RR performance.
电催化还原 CO 生成高附加值化学品为全球碳平衡提供了一条可行的途径。在此，报道了 Ni@Ni-NG(x,y=1,2,3;NG=氮掺杂石墨)的制备，其中存在 Ni 单原子位(Ni)和 Ni 纳米颗粒(Ni)。这些 Ni@Ni-NG 在 CO 还原反应(CO RR)中表现出最大 CO 法拉第效率(FE)的火山状趋势，最高点为 Ni@Ni-NG。在流动池中，Ni@Ni-NG 在-0.98 V(相对于 RHE)时表现出≈98%的最大 FE 和-264 mA cm 的大电流密度。原位实验和密度泛函理论(DFT)计算证实，Ni 和 Ni 的适当含量平衡了质子供给和 CO 加氢之间的动力学。Ni@Ni-NG 中的 Ni 促进了 H的形成，并降低了CO 加氢到*COOH 的能量势垒，并且 CO 脱附可以被 Ni 位有效地促进，从而提高了 CO RR 的性能。
