Electrochemical water splitting represents one of the most promising technologies to produce green hydrogen, which can help to realize the goal of achieving carbon neutrality. While substantial efforts on a laboratory scale have been made for understanding fundamental catalysis and developing high-performance electrocatalysts for the two half-reactions involved in water electrocatalysis, much less attention has been paid to doing relevant research on a larger scale. For example, few such researches have been done on an industrial scale. Herein, we review the very recent endeavors to bridge the gaps between fundamental research and industrial applications for water electrolysis. We begin by introducing the fundamentals of electrochemical water splitting and then present comparisons of testing protocol, figure of merit, catalyst of interest, and manufacturing cost for laboratory and industry-based water-electrolysis research. Special attention is paid to tracking the surface reconstruction process and identifying real catalytic species under different testing conditions, which highlight the significant distinctions of corresponding electrochemical reconstruction mechanisms. Advances in catalyst designs for industry-relevant water electrolysis are also summarized, which reveal the progress of moving the practical applications forward and accelerating synergies between material science and engineering. Perspectives and challenges of electrocatalyst design strategies are proposed finally to further bridge the gaps between lab-scale research and large-scale electrocatalysis applications. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/eem2.12441

Electrochemical Water Splitting: Bridging the Gaps between Fundamental Research and Industrial Applications

Theoretical calculations unveil that the formation of Os-OsSe2 heterostructures with neutralized work function (WF) perfectly balances the electronic state between strong (Os) and weak (OsSe2) adsorbents and bidirectionally optimizes the hydrogen evolution reaction (HER) activity of Os sites, significantly reducing thermodynamic energy barrier and accelerating kinetics process. Then, heterostructural Os-OsSe2 is constructed for the first time by a molten salt method and confirmed by in-depth structural characterization. Impressively, due to highly active sites endowed by the charge balance effect, Os-OsSe2 exhibits ultra-low overpotentials for HER in both acidic (26 mV @ 10 mA cm-2) and alkaline (23 mV @ 10 mA cm-2) media, surpassing commercial Pt catalysts. Moreover, the solar-to-hydrogen device assembled with Os-OsSe2 further highlights its potential application prospects. Profoundly, this special heterostructure provides a new model for rational selection of heterocomponents.

Work-function-induced Interfacial Built-in Electric Fields in Os-OsSe2 Heterostructures for Active Acidic and Alkaline Hydrogen Evolution.

Proton exchange membrane water electrolyzers (PEMWEs) are an attractive technology for renewable energy conversion and storage. By using green electricity generated from renewable sources like wind or solar, high-purity hydrogen gas can be produced in PEMWE systems, which can be used in fuel cells and other industrial sectors. To date, significant advances have been achieved in improving the efficiency of PEMWEs through the design of stack components; however, challenges remain for their large-scale and long-term application due to high cost and durability issues in acidic conditions. In this review, we examine the latest developments in engineering PEMWE systems and assess the gap that still needs to be filled for their practical applications. We provide a comprehensive summary of the reaction mechanisms, the correlation among structure-composition-performance, manufacturing methods, system design strategies, and operation protocols of advanced PEMWEs. We also highlight the discrepancies between the critical parameters required for practical PEMWEs and those reported in the literature. Finally, we propose the potential solution to bridge the gap and enable the appreciable applications of PEMWEs. This review may provide valuable insights for research communities and industry practitioners working in these fields and facilitate the development of more cost-effective and durable PEMWE systems for a sustainable energy future. 

Recent advances in proton exchange membrane water electrolysis.

The acidic oxygen evolution reaction (OER) has long been the bottleneck of proton exchange membrane water electrolyzers given its harsh oxidative and corrosive environments. Herein, we suggest an effective strategy to greatly enhance both the acidic OER activity and stability of Co3O4 spinel by atomic Ru selective substitution on the octahedral Co sites. The resulting highly symmetrical octahedral Ru-O-Co collaborative coordination with strong electron coupling effect enables the direct dioxygen radical coupling OER pathway. Indeed, both experiments and theoretical calculations reveal a thermodynamically breakthrough heterogeneous diatomic oxygen mechanism. Additionally, the active Ru-O-Co units are well-maintained upon the acidic OER thanks to the electron transfer from surrounding electron-enriched tetrahedral Co atoms via bridging oxygen bonds that suppresses the overoxidation and thus dissolution of active Ru and Co species. Consequently, the prepared catalyst, even with a low Ru mass loading of ca. 42.8 μg cm-2, exhibits an attractive acidic OER performance with a low overpotential of 200 mV and a low potential decay rate of 0.45 mV h-1 at 10 mA cm-2. Our work suggests an effective strategy to significantly enhance both the acidic OER activity and stability of low-cost electrocatalysts. 

Direct Dioxygen Radical Coupling Driven by Octahedral Ruthenium-Oxygen-Cobalt Collaborative Coordination for Acidic Oxygen Evolution Reaction.

Polymer electrolyte membrane water electrolysis (PEMWE) has been regarded as a promising technology for renewable hydrogen production. However, acidic oxygen evolution reaction (OER) catalysts with long-term stability impose a grand challenge in its large-scale industrialization. In this review, critical factors that may lead to catalyst's instability in couple with potential solutions are comprehensively discussed, including mechanical peeling, substrate corrosion, active-site over-oxidation/dissolution, reconstruction, oxide crystal structure collapse through the lattice oxygen-participated reaction pathway, etc. Last but not least, personal prospects are provided in terms of rigorous stability evaluation criteria, in situ/operando characterizations, economic feasibility and practical electrolyzer consideration, highlighting the ternary relationship of structure evolution, industrial-relevant activity and stability to serve as a roadmap towards the ultimate application of PEMWE. 

Long‐Term Stability Challenges and Opportunities in Acidic Oxygen Evolution Electrocatalysis

We report the strong catalyst-support interaction in WC-supported RuO2 nanoparticles (RuO2-WC NPs) anchored on carbon nanosheets with low loading of Ru (4.11 wt.%), which significantly promotes the oxygen evolution reaction activity with η10 of 347 mV and mass activity of 1430 A gRu-1, eight-fold higher than that of commercial RuO2 (176 A gRu-1). Theoretical calculations demonstrate that the strong catalyst-support interaction between RuO2 and WC support could optimize the surrounding electronic structure of Ru sites to reduce reaction barrier. Considering the likewise excellent catalytic ability for hydrogen production, an acidic OWS electrolyzer with good stability constructed by bifunctional RuO2-WC NPs only requires a cell voltage of 1.66 V to afford 10 mA cm-2. The unique 0D/2D nanoarchitectures rationally combined WC support with precious metal oxides provides a promising strategy to tradeoff the high catalytic activity and low cost for acidic OWS application.

Bifunctional WC-Supported RuO2 Nanoparticles for Robust Water Splitting in Acidic Media.

Strong metal-support interaction (SMSI) is a crucial concept in heterogeneous catalysis, which has been utilized to design efficient catalysts for electrocatalytic overall water splitting. Herein, a novel strong phosphide-metaphosphate interaction (SPmPI) is discovered in the RuP/CoNiP4O12 catalyst for the first time. The SPmPI leads to efficient electron transfer from RuP to CoNiP4O12 support, endowing the catalyst with a unique coordination environment of Ru-P and Ru-O, which is demonstrated to greatly facilitate the rate-determining water dissociation step. As a result, the RuP/CoNiP4O12 catalyst with proper Ru-P and Ru-O coordination numbers requires an ultralow overpotential of 27 mV to deliver a current density of 10 mA cm-2 for hydrogen evolution reaction (HER) in alkaline media. Moreover, the catalyst inherits the remarkable catalytic activity from the CoNiP4O12 support for oxygen evolution reaction (OER), and therefore is also effective for overall water splitting (requiring 1.56 V to achieve 10 mA cm-2 current density). This work not only reports a highly efficient catalyst for electrocatalytic overall water splitting, but also provides a novel concept of SPmPI for designing supported catalyst in heterogeneous catalysis. 

Strong phosphide-metaphosphate interaction in RuP/CoNiP4O12 for enhanced electrocatalytic water splitting

Surface reconstruction of Se-doped NiS2 enables high-efficiency oxygen evolution reaction

Herein, we report bifunctional molybdenum-doped nickel sulfide on nickel foam (Mo-NiSx/NF) for magnetic field-enhanced overall water splitting under alkaline conditions. Proper doping of Mo can lead to optimization of the electronic structure of NiSx, which accelerates the dissociation of H2O and the adsorption of OH− in the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) processes, respectively. In addition, the magnetically active Mo-NiSx/NF can further enhance the HER and OER activity under an applied magnetic field due to the magnetoresistance effect and the ferromagnetic (FM) exchange-field penetration effect. As a result, Mo-NiSx/NF requires low overpotentials of 307 mV at 50 mA cm−2 (for OER) and 136 mV at 10 mA cm−2 (for HER) under a magnetic field of 10000 G. Furthermore, the electrolytic cell constructed by the bifunctional Mo-NiSx/NFs as both the cathode and the anode shows a low cell voltage of 1.594 V at 10 mA cm−2 with optimal stability over 60 h under the magnetic field. Simultaneous enhancement of the HER and OER processes by an external magnetic field through rational design of electrocatalysts might be promising for overall water splitting applications. 

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/cey2.351

Magnetic field‐enhanced water splitting enabled by bifunctional molybdenum‐doped nickel sulfide on nickel foam

Encapsulating dual-phase WC-W2C nanoparticles into hollow carbon dodecahedrons for all-pH electrocatalytic hydrogen evolution

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