Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2021-11-20 , DOI: 10.1016/j.apcatb.2021.120916 Huan Zhao 1 , Dan Zhang 1, 2 , Yueyue Yuan 1 , Xueke Wu 1 , Shaoxiang Li 2 , Zhenjiang Li 3 , Jianping Lai 1 , Lei Wang 1, 2
It is an insurmountable challenge to synthesize carrier-supported ultra-small immiscible alloy catalyst with simple one-step method today. Here, we creatively report the first preparation of immiscible Ru-based alloys (RuRE-rGO NPs, RE=Gd, Er, Yb, La) with ~5 nm by solvent-free microwave reduction. Additionally, in alkaline electrocatalytic hydrogen evolution reaction (HER), RuGd-rGO NPs performed admirable (η=12 mV at 10 mA cm−2, TOF=30.6 H2 s-1 at 0.1 V), which also can be stable for 500 h even if it provides industry-related current density of 500 mA cm-2. Density functional theory further indicates that from initial to final state of the reaction, RuGd-rGO NPs have large exothermic energy (-1.34 eV), while the dissociation energy barrier of H2O is relatively low, causing the most likely occurrence of HER. This work provides sufficient space for the synthesis of ultra-small immiscible nano-alloy supported catalysts.
中文翻译:
超小型不混溶合金负载催化剂的快速大规模合成
目前用简单的一步法合成载体负载的超小型不混溶合金催化剂是一项不可逾越的挑战。在这里,我们创造性地报告了 通过无溶剂微波还原首次制备了约 5 nm的不混溶 Ru 基合金(RuRE-rGO NPs,RE=Gd,Er,Yb,La)。此外,在碱性电催化析氢反应 (HER) 中,RuGd-rGO NPs 表现出色(η=12 mV at 10 mA cm -2,TOF=30.6 H 2 s -1 at 0.1 V),也可以稳定 500 h 即使它提供 500 mA cm -2 的工业相关电流密度. 密度泛函理论进一步表明,从反应的初始状态到最终状态,RuGd-rGO NPs 具有较大的放热能(-1.34 eV),而 H 2 O的解离能垒相对较低,最有可能发生 HER。这项工作为超小型不混溶纳米合金负载催化剂的合成提供了足够的空间。