Enhancing the d/p‐Band Center Proximity with Amorphous‐Crystalline Interface Coupling for Boosted pH‐Robust Water Electrolysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(11)

Published: Jan. 26, 2023

Abstract Rationalizing non‐precious pH‐robust electrocatalysts is a crucial priority and required for multi‐scenario hydrogen production customization. Herein, an amorphous–crystalline CoBO x /NiSe heterostructure theoretically profiled constructed efficient water electrolysis. The crystalline lattice confinement induces CoCo bond shortening B‐site delocalization on amorphous , resulting in decreased d‐p band center difference (Δε ) toward the balanced intermediates adsorption/desorption. Accordingly, exhibits robust hydrogen/oxygen evolution reaction (HER/OER) catalytic activity different electrolytes. Of particular note, it achieves ultralow overpotentials both beyond‐Pt HER (14.5 mV) OER (229.1 at 10 mA cm −2 under alkaline electrolyte, reaches industrial‐level current density of 2 A . Water electrolysis stably delivered with low η voltage 1.48 V. incorporation such orbitals interface puts forward new opportunities rationally designing advanced

Language: Английский

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Ir Nanoparticles Anchored on Metal‐Organic Frameworks for Efficient Overall Water Splitting under pH‐Universal Conditions

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(17)

Published: March 2, 2023

The construction of high-activity and low-cost electrocatalysts is critical for efficient hydrogen production by water electrolysis. Herein, we developed an advanced electrocatalyst anchoring well-dispersed Ir nanoparticles on nickel metal-organic framework (MOF) Ni-NDC (NDC: 2,6-naphthalenedicarboxylic) nanosheets. Benefiting from the strong synergy between MOF through interfacial Ni-O-Ir bonds, synthesized Ir@Ni-NDC showed exceptional electrocatalytic performance evolution reaction (HER), oxygen (OER) overall splitting in a wide pH range, superior to commercial benchmarks most reported electrocatalysts. Theoretical calculations revealed that charge redistribution bridge induced optimization H2 O, OH* H* adsorption, thus leading accelerated electrochemical kinetics HER OER. This work provides new clue exploit bifunctional pH-universal splitting.

Language: Английский

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Amorphous Mo‐doped NiS_0.5Se_0.5 Nanosheets@Crystalline NiS_0.5Se_0.5 Nanorods for High Current‐density Electrocatalytic Water Splitting in Neutral Media

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 62(6)

Published: Dec. 3, 2022

Abstract It is vitally important to develop highly active, robust and low‐cost transition metal‐based electrocatalysts for overall water splitting in neutral solution especially at large current density. In this work, amorphous Mo‐doped NiS 0.5 Se nanosheets@crystalline nanorods (Am−Mo−NiS ) was synthesized using a facil one‐step strategy. phosphate buffer saline solution, the Am−Mo−NiS shows tiny overpotentials of 48 209 mV hydrogen evolution reaction (HER), 238 514 oxygen (OER) 10 1000 mA cm −2 , respectively. Moreover, delivers excellent stability least 300 h without obvious degradation. Theoretical calculations revealed that Ni sites defect‐rich structure owns higher electron state density strengthened binding energy H 2 O, which will optimize adsorption/desorption barriers reduce adsorption OER determining step.

Language: Английский

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Enabling Internal Electric Fields to Enhance Energy and Environmental Catalysis

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(11)

Published: Jan. 29, 2023

Abstract Recent years have witnessed an upsurge of interest in exploiting advanced photo‐/electrocatalysts for efficient energy conversion and environmental remediation. Constructing internal electric fields has been highlighted as a rising star to help facilitate various catalytic processes, with the merits promoting charge transfer/separation, optimizing redox potential creating effective active/adsorption sites. Internal are usually formed by polarization uneven distributions between different constituent layers, which widely exist piezoelectrics, polar surface terminations, heterostructure materials. Herein, groundbreaking interdisciplinary overview latest advances construction improve photo(electro)catalytic electrocatalytic activity is provided. This critical review begins encyclopedic summary classification, advantages, synthesis strategies fields. Subsequently, identification methods thoroughly discussed based on characterization techniques, experiments, theoretical calculations, can provide profound guidance in‐depth study To elaborate theory–structure–activity relationships fields, corresponding reaction mechanisms, modification strategies, performance jointly discussed, along discussion their practical applications. Finally, insightful analysis challenges future prospects field‐based catalysts discussed.

Language: Английский

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Advanced electrocatalysts with unusual active sites for electrochemical water splitting

InfoMat, Journal Year: 2023, Volume and Issue: 6(1)

Published: Nov. 27, 2023

Abstract Electrochemical water splitting represents a promising technology for green hydrogen production. To design advanced electrocatalysts, it is crucial to identify their active sites and interpret the relationship between structures performance. Materials extensively studied as electrocatalysts include noble‐metal‐based (e.g., Ru, Ir, Pt) non‐noble‐metal‐based 3d transition metals) compounds. Recently, advancements in characterization techniques theoretical calculations have revealed novel unusual sites. The present review highlights latest achievements discovery identification of various unconventional electrochemical splitting, with focus on state‐of‐the‐art strategies determining true establishing structure–activity relationships. Furthermore, we discuss remaining challenges future perspectives development next‐generation By presenting fresh perspective reaction involved this aims provide valuable guidance study industrial applications. image

Language: Английский

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Metastabilizing the Ruthenium Clusters by Interfacial Oxygen Vacancies for Boosted Water Splitting Electrocatalysis

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(21)

Published: Feb. 2, 2024

Abstract Metal–support interaction (MSI) is witnessed as an essential manner to stabilize active metals and tune catalytic activity for heterogonous water splitting. Kinetically driving the electrolysis (WE) appeals a rational MSI system with coupled electron‐donating/accepting (e‐D/A) characters hydrogen/oxygen evolution reactions (HER/OER). However, metal stabilization effect by will in turn restrict deblocking of e‐D/A properties challenge full electrocatalytic optimization. This study profiles heterostructure featuring metastable Ru clusters on defective NiFe hydroxide (Ru/d‐NiFe LDH) support low‐precious (≈2 wt%) platform efficient WE. It indicated that interfacial oxygen vacancies can deviate stable 4d 5 orbit 2+δ state, regulate d‐band center levels toward facilitated HER/OER processes. Resultantly, Ru/d‐NiFe LDH attains ultralow overpotentials at 10 mA cm −2 Pt‐beyond alkaline HER (18 mV) OER (220 fast kinetics durability. The symmetrical electrolyzer delivers promising voltage 1.49 V 1 m KOH seawater splitting performance. work carries interesting opportunities rationalizing sophisticated metal‐support electrocatalysts through metal‐site metastabilization engineering.

Language: Английский

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A Mini Review on Transition Metal Chalcogenides for Electrocatalytic Water Splitting: Bridging Material Design and Practical Application

Energy & Fuels, Journal Year: 2023, Volume and Issue: 37(4), P. 2608 - 2630

Published: Feb. 2, 2023

Hydrogen is believed to be one of the essential clean secondary energy sources in structure revolution both industry and daily life. Driven by renewable electricity such as solar wind power, water electrolysis for hydrogen production deemed main processes green future academia industry. Transition metal chalcogenides (TMCs) are promising candidates replace noble metals earth-abundant electrocatalysts splitting. However, it remains challenging further improve electrocatalytic activity long-term stability TMCs, especially a practical electrolyzer. This Review summarizes recent advances strategies optimizing activities TMCs toward splitting well latest investigations on surface reconstructions during electrolysis. The performances cells particularly discussed. Finally, concluding remark perspective provided, we hope inspire works this area, narrowing gap between material design application.

Language: Английский

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Stimulate the hidden catalysis potential and exposure of nickel site in NiSe@CNTs result in ultra-high HER/OER activity and stability

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 330, P. 122641 - 122641

Published: March 15, 2023

Language: Английский

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Creating Dual Active Sites in Conductive Metal‐Organic Frameworks for Efficient Water Splitting

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(20)

Published: April 7, 2023

Abstract The achievement of bifunctional metal‐organic frameworks (MOFs) remains a huge challenge due to their lack dual active sites. Herein, sites in the Co‐catecholate (Co‐CAT) are created through Ru, Ir, or Rh doping for overall water splitting. Among them, RuCo‐CAT exhibits excellent activities, outperforming benchmarked Pt/C hydrogen evolution reaction (HER) and RuO 2 oxygen (OER). theoretical calculations demonstrate that doped Ru atoms with optimal absorption energy intermediate Co centers reduced barrier rate‐determining step HER OER, respectively. Furthermore, incorporation can improve electrical conductivity capacity adsorption Co‐CAT greatly, synergistically improving activity. This strategy engineering offers novel insights into designing MOFs

Language: Английский

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Interfacial Engineering of Cobalt Thiophosphate with Strain Effect and Modulated Electron Structure for Boosting Electrocatalytic Hydrogen Evolution Reaction

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(12)

Published: Dec. 6, 2023

Abstract The fabrication of heterojunctions is an intriguing approach to boost the reactivity catalysts. However, facile preparation desirable heterojunction materials remains a challenge. Here, novel CoPS 3 /CoS 2 are created by intuitive phosphatization process on basis structurally flexible cobalt sulfide precursors. Significant stress effect exists at these heterogeneous interfaces, resulting in lattice distortions and exposure more active sites. interface interaction also modifies catalyst's electronic structure improve its electrical conductivity hydrogen adsorption capabilities. Notably, overpotential for electrocatalytic evolution reaction just 36.3 mV, which far superior those single‐component catalysts competitive with comparable reported. This work not only offers innovative electrocatalyst but strategy that can be used create based related transition metal thiophosphates.

Language: Английский

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