Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, PR China.
Guangxi Key Laboratory of Electrochemical Energy Materials, Guangxi Colleges and Universities Key Laboratory of Applied Chemistry Technology and Resource Development, School of Chemistry and Chemical Engineering, Guangxi University, Nanning 530004, PR China; Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology, Guangxi University, Nanning 530004, PR China.
J Colloid Interface Sci. 2023 Sep 15;646:361-369. doi: 10.1016/j.jcis.2023.05.006. Epub 2023 May 7.
Developing efficient and robust non-precious-metal-based hydrogen evolution reaction (HER) catalysts is highly desirable but remains quite challenging for alkaline freshwater/seawater electrolysis. In the present study, we report a theory-guided design and synthesis of a nickel foam (NF) supported N-doped carbon-coated (NC) nickel (Ni)/chromium nitride (CrN) nanosheets (NC@CrN/Ni) as a highly active and durable electrocatalyst. Our theoretical calculation firstly reveals that CrN/Ni heterostructure can greatly promote the HO dissociation via hydrogen-bond induced effect, and the N site can be optimized by hetero coupling to achieve a facile hydrogen associative desorption, thereby significantly boosting alkaline HER. Guided by theoretical calculation, we prepared the nickel-based metal-organic framework as a precursor, and introduced the Cr by the subsequent hydrothermal treatment, finally obtained the target catalyst by ammonia pyrolysis. Such a simple process ensures the exposure of abundant accessible active sites. Consequently, the as-prepared NC@CrN/Ni catalyst exhibits outstanding performance in both alkaline freshwater and seawater, with the respective overpotential of only 24 and 28 mV at a current density of 10 mA cm, respectively. More impressively, the catalyst also possesses superior durability in the constant-current test of 50 h at the different current densities of 10, 100, and 1000 mA cm.
开发高效、稳定的非贵金属基析氢反应(HER)催化剂对于碱性淡水/海水电解是非常理想的,但极具挑战性。在本研究中,我们报告了一种理论指导下的设计和合成方法,即制备了一种负载在泡沫镍(NF)上的氮掺杂碳包覆(NC)镍(Ni)/氮化铬(CrN)纳米片(NC@CrN/Ni)作为高效、稳定的电催化剂。我们的理论计算首先揭示了 CrN/Ni 异质结构可以通过氢键诱导效应极大地促进 HO 的解离,并且 N 位可以通过杂原子耦合进行优化,从而实现易于氢缔合脱附,从而显著促进碱性 HER。受理论计算的指导,我们制备了镍基金属有机框架作为前驱体,并通过随后的水热处理引入了 Cr,最后通过氨热解得到了目标催化剂。这种简单的工艺确保了大量丰富的可及活性位点的暴露。因此,所制备的 NC@CrN/Ni 催化剂在碱性淡水和海水中均表现出优异的性能,在 10 mA cm 的电流密度下,其过电势分别仅为 24 和 28 mV。更令人印象深刻的是,该催化剂在不同电流密度为 10、100 和 1000 mA cm 的恒流测试中,连续 50 小时的测试中也表现出了优异的稳定性。