Descriptor-Driven Computational Design of Bifunctional Double-Atom Hydrogen Evolution and Oxidation Reaction Electrocatalysts for Rechargeable Hydrogen Gas Batteries

Abstract

Rechargeable hydrogen gas batteries (RHGBs) have been attracting much attention as promising all-climate large-scale energy storage devices, which calls for low-cost and high-activity hydrogen evolution/oxidation reaction (HER/HOR) bifunctional electrocatalysts to replace the costly platinum-based catalysts. Based on density functional theory (DFT) computations, herein we report an effective descriptor-driven design principle to govern the HER/HOR electrocatalytic activity of double-atom catalysts (DACs) for RHGBs. We systematically investigate the d-band center variation of DACs and their correlations with HER/HOR free energies. We construct activity maps with the d-band center of DACs as a descriptor, which demonstrate that high HER/HOR electrocatalytic activity can be achieved with an appropriate d-band center of DACs. This work not only broadens the applicability of d-band center theory to the prediction of bifunctional HER/HOR electrocatalysts but also paves the way to fast screening and design of efficient and low-cost DACs to promote practical applications of RHGBs.

Efficient interfacial electron transfer induced by hollow-structured ZnIn2S4 for extending hot electron lifetimes

“…6(a), S 1 possesses the maximal Bader charge transfer (+0.57 e ), indicating the strongest reduction capacity for efficiently driving PHE as well as more rapid charge transfer dynamics. 36,37 The maximal Bader charge transfer of the S 1 site is in good agreement with its lowest Δ G * H , confirming that the S 1 site is the active site of PHE.…”

Ultrafast Thermal Synthesis of Non-Noble Metal-Based Electrocatalysts for Overall Water Splitting

“…Therefore, it is urgently required to investigate non-noble metal-based electrocatalysts, which take advantages of lowcost, earth-abundance, and highly efficient catalytic performance, even surpassing that of noble metal-based electrocatalysts. 22 Recently, a number of research studies to synthesize nonnoble metal-based electrocatalysts have been reported, which typically adopt conventional synthesis methods, such as solvothermal, 23 hydrothermal, 24 electrodeposition, 25 precipitation. 26 However, they have several drawbacks of overlong synthesis time, inaccurate control, and complicated procedures, which result in undesirable nanoparticle aggregation and throughput degradation.…”

“…In recent years, considerable effort has been devoted to reducing high overpotential, for instance, electrocatalysts based on noble metals (Pt, Ru, and Ir) have exhibited the highest catalytic activity for HER and OER. − However, the scarcity and high cost of noble metals hinder their large-scale applications. Therefore, it is urgently required to investigate non-noble metal-based electrocatalysts, which take advantages of low-cost, earth-abundance, and highly efficient catalytic performance, even surpassing that of noble metal-based electrocatalysts …”

Ultralow-Temperature Aqueous Conductive Polymer–Hydrogen Gas Battery

“…At the same time, the redox couple of hydrogen evolution and oxidation reactions (HER/HOR) exhibits a low overpotential, good stability, and fast kinetics, which makes hydrogen a highly promising reversible electrode material. Five decades passed after the traditional Ni–H 2 batteries were successfully applied to space aircraft and satellites; they have now revived thanks to the recent development of highly active hydrogen electrode catalysts. − Recently, a series of new hydrogen gas battery systems have been demonstrated, such as Mn–H 2 , lithium manganese oxide–H 2 , and iron–H 2 , all showing excellent properties of low cost, high rate, and long-term cycling stability for large-scale energy storage. Additionally, Zhu et al reported a novel aqueous proton battery that is composed of the H 2 anode and Prussian blue analogue cathode in a concentrated phosphoric acid electrolyte, achieving surprisingly low-temperature performance down to −80 °C and a stable cycle life of 1150 cycles under −60 °C.…”