Designing and constructing bifunctional electrocatalysts is vital for water splitting. Particularly, the rational interface engineering can effectively modify the active sites and promote the electronic transfer, leading to the improved splitting efficiency. Herein, free-standing and defect-rich heterogeneous MoS2/NiS2 nanosheets for overall water splitting are designed. The abundant heterogeneous interfaces in MoS2/NiS2 can not only provide rich electroactive sites but also facilitate the electron transfer, which further cooperate synergistically toward electrocatalytic reactions. Consequently, the optimal MoS2/NiS2 nanosheets show the enhanced electrocatalytic performances as bifunctional electrocatalysts for overall water splitting. This study may open up a new route for rationally constructing heterogeneous interfaces to maximize their electrochemical performances, which may help to accelerate the development of nonprecious electrocatalysts for overall water splitting.

https://onlinelibrary.wiley.com/doi/pdf/10.1002/advs.201900246

Defect-Rich Heterogeneous MoS2/NiS2 Nanosheets Electrocatalysts for Efficient Overall Water Splitting.

In electrocatalysis, doping regulation has been considered as an effective method to modulate the active sites of catalysts, providing a powerful means for creating a large variety of highly efficient catalysts for various reactions. Of particular interest, there has been growing research concerning the doping of two-dimensional transition-metal compounds (TMCs) to optimize their electrocatalytic performance. Despite the previous achievements, mechanistic insights of doping regulation in TMCs for electrocatalysis are still lacking. Herein, we provide a systematic overview of doping regulation in TMCs in terms of background, preparation, impacts on physicochemical properties, and typical applications including the hydrogen evolution reaction, oxygen evolution reaction, oxygen reduction reaction, CO2 reduction reaction, and N2 reduction reaction. Notably, we bridge the understanding between the doping regulation of catalysts and their catalytic activities via focusing on the physicochemical properties of catalysts from the aspects of vacancy concentrations, phase transformation, surface wettability, electrical conductivity, electronic band structure, local charge distribution, tunable adsorption strength, and multiple adsorption configurations. We also discuss the existing challenges and future perspectives in this promising field.

Doping regulation in transition metal compounds for electrocatalysis

Abstract Single-site cocatalysts engineered on supports offer a cost-efficient pathway to utilize precious metals, yet improving the performance further with minimal catalyst loading is still highly desirable. Here we have conducted a photochemical reaction to stabilize ultralow Pt co-catalysts (0.26 wt%) onto the basal plane of hexagonal ZnIn 2 S 4 nanosheets (Pt SS -ZIS) to form a Pt-S 3 protrusion tetrahedron coordination structure. Compared with the traditional defect-trapped Pt single-site counterparts, the protruding Pt single-sites on h -ZIS photocatalyst enhance the H 2 evolution yield rate by a factor of 2.2, which could reach 17.5 mmol g −1 h −1 under visible light irradiation. Importantly, through simple drop-casting, a thin Pt SS -ZIS film is prepared, and large amount of observable H 2 bubbles are generated, providing great potential for practical solar-light-driven H 2 production. The protruding single Pt atoms in Pt SS -ZIS could inhibit the recombination of electron-hole pairs and cause a tip effect to optimize the adsorption/desorption behavior of H through effective proton mass transfer, which synergistically promote reaction thermodynamics and kinetics. 

/pdf/protruding-pt-single-sites-on-hexagonal-znin2s4-to-3a9kccma.pdf

Protruding Pt single-sites on hexagonal ZnIn2S4 to accelerate photocatalytic hydrogen evolution

Maximizing the catalytic activity of single-atom catalysts is vital for the application of single-atom catalysts in industrial water-alkali electrolyzers, yet the modulation of the catalytic properties of single-atom catalysts remains challenging. Here, we construct strain-tunable sulphur vacancies around single-atom Ru sites for accelerating the alkaline hydrogen evolution reaction of single-atom Ru sites based on a nanoporous MoS2-based Ru single-atom catalyst. By altering the strain of this system, the synergistic effect between sulphur vacancies and Ru sites is amplified, thus changing the catalytic behavior of active sites, namely, the increased reactant density in strained sulphur vacancies and the accelerated hydrogen evolution reaction process on Ru sites. The resulting catalyst delivers an overpotential of 30 mV at a current density of 10 mA cm−2, a Tafel slope of 31 mV dec−1, and a long catalytic lifetime. This work provides an effective strategy to improve the activities of single-atom modified transition metal dichalcogenides catalysts by precise strain engineering. The modulation of single-atom catalyst properties for industrial applications remains challenging. Here, authors use strain engineering to amplify the synergistic effect between MoS2’s sulphur vacancies and single-atom Ru sites and accelerate H2 evolution electrocatalysis.

/pdf/rational-strain-engineering-of-single-atom-ruthenium-on-cfzwxqt4db.pdf

Rational strain engineering of single-atom ruthenium on nanoporous MoS2 for highly efficient hydrogen evolution.

As a potential energy carrier, hydrogen has surged up the priority list as part of broader decarbonization efforts and strategies to build or acquire clean energy economies. Driven by renewable electricity, electrochemical water splitting (WS) promises an ideal long-term, low-carbon way to produce hydrogen, with the ability to tackle various critical energy challenges. To improve the efficiency of electrocatalytic water splitting, electrocatalysts with enhanced conductivity, more exposed active sites, and high intrinsic activity are crucial for decreasing the energy gap for the rate-determining step (RDS) and subsequently improving the conversion efficiency. The incorporation of multidimensional imperfections has been demonstrated to be efficient for modulating the electron distribution and speeding up the electrocatalysis kinetics during electrocatalytic processes and this is now attracting ever-increasing attention. Herein, in this review, we summarize recent progress relating to the regulation of electrical behavior and electron distributions for the optimization of electrocatalytic water-splitting performance via defect engineering. With an emphasis on the beneficial aspects of the hydrogen economy and an in-depth understanding of electron redistribution caused by defect effects, we offer a comprehensive summary of the progress made in the last three to five years. Finally, we also offer future perspectives on the challenges and opportunities relating to water-splitting electrocatalysts in this attractive field.

Perfecting electrocatalysts via imperfections: towards the large-scale deployment of water electrolysis technology

Engineering catalytic sites at the atomic level provides an opportunity to understand the catalyst’s active sites, which is vital to the development of improved catalysts. Here we show a reliable and tunable polyoxometalate template-based synthetic strategy to atomically engineer metal doping sites onto metallic 1T-MoS2, using Anderson-type polyoxometalates as precursors. Benefiting from engineering nickel and oxygen atoms, the optimized electrocatalyst shows great enhancement in the hydrogen evolution reaction with a positive onset potential of ~ 0 V and a low overpotential of −46 mV in alkaline electrolyte, comparable to platinum-based catalysts. First-principles calculations reveal co-doping nickel and oxygen into 1T-MoS2 assists the process of water dissociation and hydrogen generation from their intermediate states. This research will expand on the ability to improve the activities of various catalysts by precisely engineering atomic activation sites to achieve significant electronic modulations and improve atomic utilization efficiencies. While heterogeneous catalysts can act as tangible, efficient materials for energy conversion, understanding the active catalytic sites is challenging. Here, authors engineer specific catalytic sites into molybdenum sulfide to improve and elucidate hydrogen evolution electrocatalysis.

/pdf/atomically-engineering-activation-sites-onto-metallic-1t-mos-2qchqw3k4m.pdf

Atomically engineering activation sites onto metallic 1T-MoS 2 catalysts for enhanced electrochemical hydrogen evolution.

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

/pdf/publisher-correction-atomically-engineering-activation-sites-5fki7jol18.pdf

Publisher Correction: Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution.

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Atomically engineering activation sites onto metallic 1T-MoS 2 catalysts for enhanced electrochemical hydrogen evolution.

Publisher Correction: Atomically engineering activation sites onto metallic 1T-MoS2 catalysts for enhanced electrochemical hydrogen evolution.