School of Chemistry, UNSW Materials and Manufacturing Futures Institute, The University of New South Wales, Sydney, New South Wales, 2052, Australia.
Engineering Research Center of Advanced Functional Material Manufacturing of Ministry of Education, Zhengzhou University, Zhengzhou, 450001, China.
Nat Commun. 2023 Feb 1;14(1):547. doi: 10.1038/s41467-023-36100-3.
Electrocatalytic synergy is a functional yet underrated concept in electrocatalysis. Often, it materializes as intermetallic interaction between different metals. We demonstrate interphasic synergy in monometallic structures is as much effective. An interphasic synergy between Ni(OH) and Ni-N/Ni-C phases is reported for alkaline hydrogen evolution reaction that lowers the energy barriers for hydrogen adsorption-desorption and facilitates that of hydroxyl intermediates. This makes ready-to-serve Ni active sites and allocates a large amount of Ni d-states at Fermi level to promote charge redistribution from Ni(OH) to Ni-N/Ni-C and the co-adsorption of H and OH intermediates on Ni-N/Ni-C moieties. As a result, a Ni(OH)@Ni-N/Ni-C hetero-hierarchical nanostructure is developed, lowering the overpotentials to deliver -10 and -100 mA cm in alkaline media by 102 and 113 mV, respectively, compared to monophasic Ni(OH) catalyst. This study unveils the interphasic synergy as an effective strategy to design monometallic electrocatalysts for water splitting and other energy applications.
电催化协同作用是电催化中一个很有意义但尚未得到充分重视的概念。通常,它表现为不同金属之间的金属间相互作用。我们证明了在单相结构中也存在相间协同作用。在碱性析氢反应中,报道了 Ni(OH)和 Ni-N/Ni-C 相之间的相间协同作用,降低了氢吸附-解吸的能量势垒,并促进了羟基中间体的形成。这使得 Ni 活性位点随时可用,并在费米能级处分配大量的 Ni d 态,以促进从 Ni(OH)到 Ni-N/Ni-C 的电荷重新分布,以及 H 和 OH 中间体在 Ni-N/Ni-C 部分上的共吸附。结果,开发了 Ni(OH)@Ni-N/Ni-C 异质分层纳米结构,与单相 Ni(OH)催化剂相比,在碱性介质中分别将 -10 和 -100 mA cm 的过电位降低了 102 和 113 mV。这项研究揭示了相间协同作用是设计用于水分解和其他能源应用的单相电催化剂的有效策略。