The Electronic Metal–Support Interaction Directing the Design of Single Atomic Site Catalysts: Achieving High Efficiency Towards Hydrogen Evolution

Abstract

It is still of great difficulty to develop the non‐platinum catalyst with high catalytic efficiency towards hydrogen evolution reaction via the strategies till now. Therefore, it is necessary to develop the new methods of catalyst designing. Here, we put forward the catalyst designed by the electronic metal–support interaction (EMSI), which is demonstrated to be a reliable strategy to find out the high‐efficiency catalyst. We carried out the density functional theory calculation first to design the proper EMSI of the catalyst. We applied the model of M1‐M2‐X (X=C, N, O) during the calculation. Among the catalysts we chose, the EMSI of Rh1TiC, with the active sites of Rh1‐Ti2C2, is found to be the most proper one for HER. The electrochemical experiment further demonstrated the feasibility of the EMSI strategy. The single atomic site catalyst of Rh1‐TiC exhibits higher catalytic efficiency than that of state‐of‐art Pt/C. It achieves a small overpotential of 22 mV and 86 mV at the at the current density of 10 mA cm−2 and 100 mA cm−2 in acid media, with a Tafel slope of 25 mV dec−1 and a mass activity of 54403.9 mA cm−2 mgRh−1 (vs. 192.2 mA cm−2 mgPt−1 of Pt/C). Besides, it also shows appealing advantage in energy saving compared with Pt/C (≈20 % electricity consuming decrease at 2 kA m−2) Therefore, we believe that the strategy of regulating EMSI can act as a possible way for achieving the high catalytic efficiency on the next step of SACs.

Activation of Main‐Group Antimony Atomic Sites for Oxygen Reduction Catalysis

“…The obvious quantum size effect and maximized utilization of active atoms are the outstanding advantages of SACs to compete with traditional catalysts [4–6] . Hence, they are attracting a broad interest from a variety of fields, involving energy conversation and storage, [7] industrial catalytic reactions, [8] and in particular, electrocatalysis [9–11] . Till now, lots of transition‐metal SACs have been reported to be successfully applied as electrocatalysts for the oxygen reduction reaction (ORR) [12, 13] .…”

Single-atom catalysts: stimulating electrochemical CO2 reduction reaction in the industrial era

“…Different from the characteristics of inert carbon substrates, nanocrystals typically have high catalytic activity, which modify the single metallic atoms at the interface and can regulate the local electron density at the active centers. [73][74][75][76][77][78] The impregnation method is a general strategy to synthesize nanocrystal/cluster-supported SACs, which is different from carbon-supported SACs, where galvanic replacement (GR) 79,80 and cation/anion exchange reaction 81,82 can occur on nanocrystals/clusters. Zheng et al developed a method to deposit single Pd atoms on the (100) and (110) facets of Cu nanocrystals through a GR reaction.…”

Investigation of the Stability and Hydrogen Evolution Activity of Dual-Atom Catalysts on Nitrogen-Doped Graphene

“…Single atom catalysts (SACs) exhibit the maximum atomic efficiency, high selectivity, and high activity towards a variety of chemical reactions, which opens up a new frontier in the field of catalysis [ 1 , 2 , 3 , 4 ]. However, the practical chemical processes require a huge number of SACs, which make them easy to aggregate and form clusters owing to their high surface energies [ 5 ].…”