Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-12-27 , DOI: 10.1016/j.apcatb.2022.122331 Dewen Wang , Dongxu Jiao , Ming Gong , Huafeng Fan , Yuting Chen , Lezhi Wang , Jinchang Fan , Jiandong Wu , David J. Singh , Jingxiang Zhao , Weitao Zheng , Xiaoqiang Cui
Single-atom catalysts have attracted extensive attention due to their unique performances and high atom utilization. However, is single atom always the best? Here we found a reverse case that nickel metaphosphate (NPO) supported nanoparticles (Run) is much better than single atoms (Rus) for all pH hydrogen evolution. The mass activity of Run-NPO is 3.8 times higher than that of Rus-NPO, and 21.4 times higher than that of Pt/C in alkaline media. The results show that Ru nanoparticle possess lower valence state than single atom, providing optimized Ru-H bond strength and suitable hydrogen adsorption free energy. As a novel support, NPO is also essential for firmly anchoring Ru and transporting electrons for optimizing the d-band center, and eventually accelerating the H2O dissociation in rate-limiting Volmer step. This work gives Ru-NPO promising potential for practical hydrogen production, and sheds light on the exploration of supported metal catalysts in energy conversion-related fields.
中文翻译:
偏磷酸镍支持钌用于所有 pH 析氢:从单原子、簇到纳米粒子
单原子催化剂由于其独特的性能和较高的原子利用率而受到广泛关注。然而,单原子总是最好的吗?在这里,我们发现了一个相反的情况,即偏磷酸镍 (NPO) 支持的纳米粒子 (Ru n )在所有 pH 析氢方面都比单个原子 (Ru s )好得多。Ru n -NPO在碱性介质中的质量活度比Ru s -NPO高3.8倍,比Pt/C高21.4倍。结果表明,Ru 纳米粒子具有比单个原子更低的价态,提供优化的 Ru-H 键强度和合适的氢吸附自由能。作为一种新型支持,NPO 对于牢固锚定 Ru 和传输电子以优化d带中心,并最终在限速 Volmer 步骤中加速 H 2 O 解离。这项工作为 Ru-NPO 在实际制氢方面提供了广阔的前景,并为在能量转换相关领域探索负载型金属催化剂提供了思路。