Importing Atomic Rare‐Earth Sites to Activate Lattice Oxygen of Spinel Oxides for Electrocatalytic Oxygen Evolution DOI Creative Commons
Xuan Wang,

Jinrui Hu,

Tingyu Lu

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 9, 2024

Abstract Spinel oxides have emerged as highly active catalysts for the oxygen evolution reaction (OER). Owing to covalency competition, OER process on spinel often follows an arduous adsorbate mechanism (AEM) pathway. Herein, we propose a novel rare‐earth sites substitution strategy tune lattice redox of and bypass AEM scaling relationship limitation. Taking NiCo 2 O 4 model, incorporation Ce into octahedral site induces formation Ce−O−M (M=Ni, Co) bridge, which triggers charge redistribution within . The developed Ce−NiCo exhibits remarkable activity with low overpotential, satisfactory electrochemical stability, good practicability in anion‐exchange membrane water electrolyzer. Theoretical analyses reveal that surface more favorable (LOM) pathway non‐concerted proton‐electron transfers compared pure , also verified by pH‐dependent behavior situ Raman analysis. 18 O‐labeled mass spectrometry provides direct evidence released during originates from We discover electron delocalization f states through favoring antibonding state occupation Ni−O bonding [Ce−O−Ni] unit site, thereby activating OER. This work new perspective designing offers significant insights rare‐earth‐enhanced LOM mechanism.

Language: Английский

Bifunctional Electrocatalysts for Overall and Hybrid Water Splitting DOI
Quan Li, Hui Jiang,

Guoliang Mei

et al.

Chemical Reviews, Journal Year: 2024, Volume and Issue: 124(7), P. 3694 - 3812

Published: March 22, 2024

Electrocatalytic water splitting driven by renewable electricity has been recognized as a promising approach for green hydrogen production. Different from conventional strategies in developing electrocatalysts the two half-reactions of (e.g., and oxygen evolution reactions, HER OER) separately, there growing interest designing bifunctional electrocatalysts, which are able to catalyze both OER. In addition, considering high overpotentials required OER while limited value produced oxygen, is another rapidly exploring alternative oxidation reactions replace hybrid toward energy-efficient generation. This Review begins with an introduction on fundamental aspects splitting, followed thorough discussion various physicochemical characterization techniques that frequently employed probing active sites, emphasis reconstruction during redox electrolysis. The design, synthesis, performance diverse based noble metals, nonprecious metal-free nanocarbons, overall acidic alkaline electrolytes, thoroughly summarized compared. Next, their application also presented, wherein anodic include sacrificing agents oxidation, pollutants oxidative degradation, organics upgrading. Finally, concise statement current challenges future opportunities presented hope guiding endeavors quest sustainable

Language: Английский

Citations

229
Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

213
Valence Oscillation of Ru Active Sites for Efficient and Robust Acidic Water Oxidation DOI
Liming Deng, Sung‐Fu Hung,

Zih‐Yi Lin

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(48)

Published: Sept. 6, 2023

The continuous oxidation and leachability of active sites in Ru-based catalysts hinder practical application proton-exchange membrane water electrolyzers (PEMWE). Herein, robust inter-doped tungsten-ruthenium oxide heterostructures [(Ru-W)Ox ] fabricated by sequential rapid metal thermomigration processes are proposed to enhance the activity stability acidic oxygen evolution reaction (OER). introduction high-valent W species induces valence oscillation Ru during OER, facilitating cyclic transition states maintaining operation sites. preferential electronic gain heterostructure significantly stabilize RuOx on WOx substrates beyond Pourbaix limit bare RuO2 . Furthermore, asymmetric Ru-O-W units generated around interface adsorb intermediates synergistically, enhancing intrinsic OER activity. Consequently, (Ru-W)Ox not only demonstrate an overpotential 170 mV at 10 mA cm-2 excellent 300 h electrolytes but also exhibit potential for applications, as evidenced stable 0.5 A PEMWE.

Language: Английский

Citations

139
Advanced electrocatalysts with unusual active sites for electrochemical water splitting DOI Creative Commons
Hainan Sun, Xiaomin Xu, Hyunseung Kim

et al.

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

Citations

95
Lanthanide-regulating Ru-O covalency optimizes acidic oxygen evolution electrocatalysis DOI Creative Commons
Lu Li, Gengwei Zhang, Chenhui Zhou

et al.

Nature Communications, Journal Year: 2024, Volume and Issue: 15(1)

Published: June 11, 2024

Abstract Precisely modulating the Ru-O covalency in RuO x for enhanced stability proton exchange membrane water electrolysis is highly desired. However, transition metals with d -valence electrons, which were doped into or alloyed , are inherently susceptible to influence of coordination environment, making it challenging modulate a precise and continuous manner. Here, we first deduce that introduction lanthanide gradually changing electronic configurations can continuously owing shielding effect 5 s /5 p orbitals. Theoretical calculations confirm durability Ln-RuO following volcanic trend as function covalency. Among various Er-RuO identified optimal catalyst possesses 35.5 times higher than 2 . Particularly, -based device requires only 1.837 V reach 3 A cm −2 shows long-term at 500 mA 100 h degradation rate mere 37 μV −1

Language: Английский

Citations

76
Ru/Ir‐Based Electrocatalysts for Oxygen Evolution Reaction in Acidic Conditions: From Mechanisms, Optimizations to Challenges DOI Creative Commons
Rong Qin, Guanzhen Chen,

Caihong Feng

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(21)

Published: March 19, 2024

Abstract The generation of green hydrogen by water splitting is identified as a key strategic energy technology, and proton exchange membrane electrolysis (PEMWE) one the desirable technologies for converting renewable sources into hydrogen. However, harsh anode environment PEMWE oxygen evolution reaction (OER) involving four‐electron transfer result in large overpotential, which limits overall efficiency production, thus efficient electrocatalysts are needed to overcome high overpotential slow kinetic process. In recent years, noble metal‐based (e.g., Ru/Ir‐based metal/oxide electrocatalysts) have received much attention due their unique catalytic properties, already become dominant acidic OER process applied commercial devices. these still face thorny problem conflicting performance cost. this review, first, metal briefly classified according forms existence, mechanisms outlined. Then, focus on summarizing improvement strategies with respect activity stability over years. Finally, challenges development prospects discussed.

Language: Английский

Citations

71
RuO2–CeO2 Lattice Matching Strategy Enables Robust Water Oxidation Electrocatalysis in Acidic Media via Two Distinct Oxygen Evolution Mechanisms DOI
Haoqiang Song, Xue Yong, Geoffrey I. N. Waterhouse

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(5), P. 3298 - 3307

Published: Feb. 15, 2024

The discovery of acid-stable and highly active electrocatalysts for the oxygen evolution reaction (OER) is crucial in quest high-performance water-splitting technologies. Herein, a heterostructured RuO2–CeO2 electrocatalyst was constructed by using lattice-matching strategy. interfacial Ru–O–Ce bridge structure provided channel electron transfer between Ru Ce, creating lattice stress that distorts local RuO2. resulting catalyst exhibited attractive stability with negligible decay after 1000 h OER 0.5 M H2SO4, along high activity an overpotential only 180 mV at 10 mA cm–2. In situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS), differential electrochemical mass spectrometry (DEMS), density functional theory (DFT) calculations were used to reveal interface noninterface RuO2 sites enabled oxide path mechanism (OPM) enhanced adsorbate (AEM-plus), respectively, during OER. simultaneous independent pathways accessible matching guides improved design acidic media.

Language: Английский

Citations

70
Unraveling Quantum Mysteries: Probing the Interplay of CdS Quantum Dots and g-C3N4 Nanosheets for Enhanced Photo/Electrocatalytic Hydrogen Evolution DOI
Amir Mehtab, Pravin P. Ingole, Jahangeer Ahmed

et al.

The Journal of Physical Chemistry C, Journal Year: 2023, Volume and Issue: 128(1), P. 85 - 94

Published: Dec. 27, 2023

A series of CdS quantum dots (QDs) at low temperature were grown on the nanosheets (NSs) g-C3N4 through an in situ successive ionic layer adsorption and reaction process. The visible light active band gap ultrathin NSs has attracted more attention due to its essential bandgap for water splitting reaction. However, a single catalyst with limited number sites does not exhibit significant photo/electrocatalytic activity hydrogen production. In current strategies, development photogenerated charge transfer-driven type-II QDs/g-C3N4 heterostructure demonstrates enhanced evolution amount 14.8 mmol gcat–1 H2 gas AQY 27.6% as result decreased transfer resistance significantly increased electrochemical surface area. Additionally, as-prepared shown overpotentials 182 382 mV (HER) oxygen (OER) reactions reach density 10 mA cm–2, respectively. addition, bifunctional electrocatalyst exhibits 4- 6-fold higher mass material OER HER compared g-C3N4, considerable faradaic efficiency under potentiostatic system, Moreover, remarkable was well explained photoluminescence quenching effect Mott–Schottky analysis.

Language: Английский

Citations

60
Iron Oxyhydroxide: Structure and Applications in Electrocatalytic Oxygen Evolution Reaction DOI

Bingrong Guo,

Haohao Huo,

Qixuan Zhuang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(25)

Published: March 10, 2023

Abstract Oxygen evolution reaction (OER) is the anodic half‐reaction for crucial energy devices, such as water electrolysis, metal–air battery, and electrochemical CO 2 reduction. Fe‐based materials are recognized one of most promising electrocatalysts OER because its extremely low price high activity. In particular, iron oxyhydroxide (FeOOH) not only highly active toward OER, but also widely accepted true species plenty converted into FeOOH during test. Herein, recent advances FeOOH‐based nano‐structure application in reviewed. The relationship between structure catalytic performance, followed by introduction current strategies enhancing activity (i.e., crystalline phase engineering, element doping, construction hybrid materials) mainly focused. Finally, a summary perspective about remaining challenges future opportunities this area further design provided.

Language: Английский

Citations

59
Next-Generation Green Hydrogen: Progress and Perspective from Electricity, Catalyst to Electrolyte in Electrocatalytic Water Splitting DOI Creative Commons
Xueqing Gao, Yutong Chen,

Yujun Wang

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: July 5, 2024

Green hydrogen from electrolysis of water has attracted widespread attention as a renewable power source. Among several production methods, it become the most promising technology. However, there is no large-scale system currently that can compete with conventional fossil fuel production. Renewable energy electrocatalytic splitting an ideal technology environmental cleanliness protection and good purity, which meet requirements future development. This review summarizes introduces current status by three aspects: electricity, catalyst electrolyte. In particular, present situation latest progress key sources power, catalytic materials electrolyzers for are introduced. Finally, problems generation electrolytic directions next-generation green in discussed outlooked. It expected this will have important impact on field water.

Language: Английский

Citations

52