Abstract:Development of robust catalysts for electrochemical water splitting is a critical topic for the energy conversion field. Herein, a precise electrochemical reconstruction of IrTe 2 hollow nanoshuttles (HNSs) is performed for oxygen and hydrogen evolution reactions (OER and HER), the two half reactions of water splitting. It is determined that the reconstruction of IrTe 2 HNSs can be regulated by adjusting the potential during electrochemical dealloying, in which mild and high potentials lead to the formation of… Show more
“…[ 18 ] From this viewpoint, an energy favorable surface reconstruction process during the initial stage can significantly accelerate the catalytic kinetics and contribute to generate stable active sites, and thus considerably enhancing the OER performance. [ 19 ] It has reported that a low activation energy barrier for initiating surface reconstruction is crucial for achieving rapid and stable OER, [ 20 ] and the level of difficulty of the initiation of the surface reconstruction can be read from the onset overpotential of the catalysts, in which a lower onset overpotential means a lower energy barrier for surface reconstruction. [ 21 ] A rapid low‐barrier surface reconstruction can achieve rapid creation and stabilization of active centers for following long‐time operation, can reduce the whole energy consumption during the electrocatalysis, and enhance the overall reaction stability, which are highly desired for industrial‐scale production.…”
It has been well recognized that the surface reconstruction of electrocatalysts at the initial stage in the form of phase transitions, defect migrations, valence regulations, etc., plays a critical role in generating real, surface active catalytic centers and achieving steady surface reactions. It is also expected that a low activation energy barrier for initiating surface reconstruction is crucial for rapid and stable electrochemical catalysis. Despite this, the surface reconstruction kinetics and their effects on catalytic reactions have been rarely investigated. Herein, using phase modulated polymorphic cobalt‐based catalysts with tailorable nitrogen‐metal bonds through a cationic molybdenum‐substitution strategy, real‐time X‐ray photoelectron spectroscopy (XPS) structural monitoring of the surface chemical state evolution during the catalytic reaction is performed to track the initial surface reconstruction kinetics during the alkaline oxygen evolution reaction (OER). It is concluded that the molybdenum‐modulated cobalt‐based nanocatalyst can be tuned with favorable initial surface reconstruction and stabilized active centers to reach optimized OER catalysis, accompanied by a low onset overpotential of only 210 mV and a favorable overpotential at 10 mA cm–2 of 290 mV, outperforming the commercial, noble‐metallic RuO2 catalyst. This study thus provides new conceptual insights into rationally regulating the initial surface reconstruction kinetics for high‐performance electrocatalysis reactions.
“…[ 18 ] From this viewpoint, an energy favorable surface reconstruction process during the initial stage can significantly accelerate the catalytic kinetics and contribute to generate stable active sites, and thus considerably enhancing the OER performance. [ 19 ] It has reported that a low activation energy barrier for initiating surface reconstruction is crucial for achieving rapid and stable OER, [ 20 ] and the level of difficulty of the initiation of the surface reconstruction can be read from the onset overpotential of the catalysts, in which a lower onset overpotential means a lower energy barrier for surface reconstruction. [ 21 ] A rapid low‐barrier surface reconstruction can achieve rapid creation and stabilization of active centers for following long‐time operation, can reduce the whole energy consumption during the electrocatalysis, and enhance the overall reaction stability, which are highly desired for industrial‐scale production.…”
It has been well recognized that the surface reconstruction of electrocatalysts at the initial stage in the form of phase transitions, defect migrations, valence regulations, etc., plays a critical role in generating real, surface active catalytic centers and achieving steady surface reactions. It is also expected that a low activation energy barrier for initiating surface reconstruction is crucial for rapid and stable electrochemical catalysis. Despite this, the surface reconstruction kinetics and their effects on catalytic reactions have been rarely investigated. Herein, using phase modulated polymorphic cobalt‐based catalysts with tailorable nitrogen‐metal bonds through a cationic molybdenum‐substitution strategy, real‐time X‐ray photoelectron spectroscopy (XPS) structural monitoring of the surface chemical state evolution during the catalytic reaction is performed to track the initial surface reconstruction kinetics during the alkaline oxygen evolution reaction (OER). It is concluded that the molybdenum‐modulated cobalt‐based nanocatalyst can be tuned with favorable initial surface reconstruction and stabilized active centers to reach optimized OER catalysis, accompanied by a low onset overpotential of only 210 mV and a favorable overpotential at 10 mA cm–2 of 290 mV, outperforming the commercial, noble‐metallic RuO2 catalyst. This study thus provides new conceptual insights into rationally regulating the initial surface reconstruction kinetics for high‐performance electrocatalysis reactions.
“…[4,9,13] Ir-based composites with different morphologies have been developed and investigated as potential OER catalysts. [14,15,16] However, Ir cannot be efficiently used at a large scale because of its high cost, scarcity, and poor durability. Designing an Ir-based catalyst with a low loading, high mass specific activity, and adequate stability can solve these drawbacks; however, the activity of such catalyst would be hindered by the presence of unstable active Water electrolysis, which is a promising high-purity H 2 production method, lacks pH-universality; moreover, highly efficient electrocatalysts that accelerate the sluggish anodic oxygen evolution reaction (OER) are scarce.…”
Section: Introductionmentioning
confidence: 99%
“…Moreover, when paired with commercial 20 wt% Pt/C, P-IrO x @ DG can deliver current densities of 350.0, 317.6, and 47.1 mA cm −2 sites and unfavorable reconstruction during operation. [16][17][18] Embedding Ir by conductive carbon substrates like graphene and carbon nanotubes may improve the catalytic stability and intrinsic activity. [19] High-temperature pyrolysis and hydrothermal/solvothermal processes are commonly used to prepare metal composite/carbon hybrids.…”
Water electrolysis, which is a promising high‐purity H2 production method, lacks pH‐universality; moreover, highly efficient electrocatalysts that accelerate the sluggish anodic oxygen evolution reaction (OER) are scarce. Geometric structure engineering and electronic structure modulation can be efficiently used to improve catalyst activity. Herein, a facile Ar plasma treatment method to fabricate a composite of uniformly dispersed iridium‐copper oxide nanoclusters supported on defective graphene (DG) to form IrCuOx@DG, is described. Acid leaching can be used to remove Cu atoms and generate porous IrOx nanoclusters supported on DG (P–IrOx@DG), which can serve as efficient and robust pH‐universal OER electrocatalysts. Moreover, when paired with commercial 20 wt% Pt/C, P–IrOx@DG can deliver current densities of 350.0, 317.6, and 47.1 mA cm−2 at a cell voltage of 2.2 V for overall water splitting in 0.5 m sulfuric acid, 1.0 m potassium hydroxide, and 1.0 m phosphate buffer solution, respectively, outperforming commercial IrO2 and nonporous IrOx nanoclusters supported on DG (O–IrOx@DG). Probing experiment, X‐ray absorption spectroscopy, and theoretical calculation results demonstrate that Cu removal can successfully create P–IrOx nanoclusters and introduce unsaturated Ir atoms. The optimum binding energies of oxygenated intermediate species on unsaturated Ir sites and ultrafine IrOx nanoclusters contribute to the high intrinsic OER catalytic activity of P–IrOx@DG.
“…Ru/Ir‐based precious metal materials are deemed as the most excellent OER electrocatalysts, but their large‐scale applications are limited by their high cost and scarcity [5] . Therefore, it is necessary to develop high‐performance and earth‐abundant non‐noble metal catalysts for OER for industrial applications [4a,6] …”
Herein, a transition metal dissolution‐oxygen vacancy strategy, based on dissolution of highly oxidized transition metal species in alkaline electrolyte, was suggested to construct a high‐performance amorphous Co(OH)2/WOx (a‐CoW) catalyst for the oxygen evolution reaction (OER). The surface reconstruction of a‐CoW and its evolution were described by regulating oxygen vacancies. With continuous dissolution of W species, oxygen vacancies on the surface were generated rapidly, the surface reconstruction was promoted, and the OER performance was improved significantly. During the surface reconstruction, W species also played a role in electronic modulation for Co. Due to its rapid surface reconstruction, a‐CoW exhibited excellent OER performance in alkaline electrolyte with an overpotential of 208 mV at 10 mA cm−2 and had long‐term stability for at least 120 h. This work shows that the transition metal dissolution‐oxygen vacancy strategy is effective for preparation of high‐performance catalysts.
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