Materials Containing Single‐, Di‐, Tri‐, and Multi‐Metal Atoms Bonded to C, N, S, P, B, and O Species as Advanced Catalysts for Energy, Sensor, and Biomedical Applications DOI Creative Commons
Jitendra N. Tiwari, Krishan Kumar, Moein Safarkhani

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(33)

Published: July 1, 2024

Abstract Modifying the coordination or local environments of single‐, di‐, tri‐, and multi‐metal atom (SMA/DMA/TMA/MMA)‐based materials is one best strategies for increasing catalytic activities, selectivity, long‐term durability these materials. Advanced sheet supported by metal atom‐based have become a critical topic in fields renewable energy conversion systems, storage devices, sensors, biomedicine owing to maximum utilization efficiency, precisely located centers, specific electron configurations, unique reactivity, precise chemical tunability. Several offer excellent support are attractive applications energy, medical research, such as oxygen reduction, production, hydrogen generation, fuel selective detection, enzymatic reactions. The strong metal–metal metal–carbon with metal–heteroatom (i.e., N, S, P, B, O) bonds stabilize optimize electronic structures atoms due interfacial interactions, yielding activities. These provide models understanding fundamental problems multistep This review summarizes substrate structure‐activity relationship different active sites based on experimental theoretical data. Additionally, new synthesis procedures, physicochemical characterizations, biomedical discussed. Finally, remaining challenges developing efficient SMA/DMA/TMA/MMA‐based presented.

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
Defect engineering of two-dimensional materials for advanced energy conversion and storage DOI
Fu Liu, Zhanxi Fan

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(5), P. 1723 - 1772

Published: Jan. 1, 2023

Defective two-dimensional (2D) materials show huge potential for energy-related fields. This review overviews the formation/evolution mechanisms and engineering strategies of defects in 2D materials, which enable enhanced electrode reaction kinetics.

Language: Английский

Citations

196
In Situ Synthesis of Chemically Bonded 2D/2D Covalent Organic Frameworks/O‐Vacancy WO3 Z‐Scheme Heterostructure for Photocatalytic Overall Water Splitting DOI

Rongchen Shen,

Guijie Liang,

Lei Hao

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(33)

Published: June 15, 2023

Abstract Covalent organic frameworks (COFs) have shown great promise for photocatalytic hydrogen evolution via water splitting. However, the four‐electron oxidation of remains elusive toward oxygen evolution. Enabling this pathway is critical to improve yield and maximize atom utilization efficiency. A Z‐scheme heterojunction proposed overcoming fundamental issues in COF‐based overall splitting (OWS), such as inefficient light absorption, charge recombination, poor ability. It that construction a novel 2D/2D through situ growth COFs on O‐vacancy WO 3 nanosheets (Ov‐WO ) WOC chemical bond can remarkably promote OWS. Benefiting from synergistic effect between enhanced built‐in electric field by interfacial bond, strong ability Ov‐WO 3, ultrathin structure TSCOF, both separation efficiency photogenerated electron–hole pairs be significantly enhanced. An impressive half‐rection rate 593 mmol h −1 g 146 (hydrogen) 68 (oxygen) µmol are achieved COF‐WO (TSCOFW) composite. This with two‐step excitation precisely cascaded charge‐transfer makes it responsible efficient solar‐driven OWS without sacrificial agent.

Language: Английский

Citations

122
Defect Engineered Metal–Organic Framework with Accelerated Structural Transformation for Efficient Oxygen Evolution Reaction DOI Open Access

Jieting Ding,

Danyu Guo,

Nanshu Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(43)

Published: Sept. 6, 2023

Metal-organic frameworks (MOFs) have been increasingly applied in oxygen evolution reaction (OER), and the surface of MOFs usually undergoes structural transformation to form metal oxyhydroxides serve as catalytically active sites. However, controllable regulation reconstruction process remains a great challenge. Here we report defect engineering strategy facilitate during OER with enhanced activity. Defective (denoted NiFc'x Fc1-x ) abundant unsaturated sites are constructed by mixing ligands 1,1'-ferrocene dicarboxylic acid (Fc') defective ferrocene carboxylic (Fc). series more prone be transformed compared non-defective (NiFc'). Moreover, as-formed derived from contain vacancies. NiFc'Fc grown on nickel foam exhibits excellent catalytic activity an overpotential 213 mV at current density 100 mA cm-2 , superior that undefective NiFc'. Experimental results theoretical calculations suggest vacancies adsorption oxygen-containing intermediates centers, thus significantly improving

Language: Английский

Citations

117
Coupling Adsorbed Evolution and Lattice Oxygen Mechanism in Fe‐Co(OH)2/Fe2O3 Heterostructure for Enhanced Electrochemical Water Oxidation DOI Creative Commons

Sisi Xin,

Yu Tang, Baohua Jia

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(45)

Published: Sept. 1, 2023

Abstract Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water‐splitting to generate hydrogen. However, the traditional adsorbed mechanism (AEM) possesses sluggish kinetics due scaling relationship, while lattice oxygen (LOM) triggers an unstable structure escaping of oxygen. Herein, proof‐of‐concept Fe‐Co(OH) 2 /Fe O 3 heterostructure is put forward, where following AEM can complete rapidly deprotonation process Fe LOM trigger O─O coupling step. Combining theoretical and experimental investigation confirmed that redistributed space‐charge junction optimize synergistically oxygen, facilitate synchronously OER activity stability. As result, shows excellent performance with low overpotential only 219 249 mV reach current density 10 100 mA cm −2 . Specifically, electrocatalyst maintains long‐term stability h at large This work paves avenue break through limit conventional mechanism.

Language: Английский

Citations

116
Manipulating electron redistribution induced by asymmetric coordination for electrocatalytic water oxidation at a high current density DOI
Sheng Zhao, Feng Hu, Lijie Yin

et al.

Science Bulletin, Journal Year: 2023, Volume and Issue: 68(13), P. 1389 - 1398

Published: June 3, 2023

Language: Английский

Citations

98
Ir Single Atoms Boost Metal–Oxygen Covalency on Selenide-Derived NiOOH for Direct Intramolecular Oxygen Coupling DOI
Zhao-Hua Yin,

Yuan Huang,

Kepeng Song

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(10), P. 6846 - 6855

Published: Feb. 29, 2024

This investigation probes the intricate interplay of catalyst dynamics and reaction pathways during oxygen evolution (OER), highlighting significance atomic-level local ligand structure insights in crafting highly active electrocatalysts. Leveraging a tailored ion exchange followed by electrochemical dynamic reconstruction, we engineered novel catalytic featuring single Ir atoms anchored to NiOOH (Ir1@NiOOH). approach involved strategic replacement Fe with Ir, facilitating transition selenide precatalysts into (oxy)hydroxides. elemental substitution promoted an upward shift O 2p band intensified metal–oxygen covalency, thereby altering OER mechanism toward enhanced activity. The from single-metal site (SMSM) dual-metal-site (DMSM) Ir1@NiOOH was substantiated situ differential mass spectrometry (DEMS) supported theoretical insights. Remarkably, electrode exhibited exceptional electrocatalytic performance, achieving overpotentials as low 142 308 mV at current densities 10 1000 mA cm–2, respectively, setting new benchmark for electrocatalysis OER.

Language: Английский

Citations

97
A Monolayer High‐Entropy Layered Hydroxide Frame for Efficient Oxygen Evolution Reaction DOI
Yiran Ding, Zhouyang Wang,

Zijia Liang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: unknown

Published: June 7, 2023

Abstract High‐entropy materials with tailored geometric and elemental compositions provide a guideline for designing advanced electrocatalysts. Layered double hydroxides (LDHs) are the most efficient oxygen evolution reaction (OER) catalyst. However, due to huge difference in ionic solubility product, an extremely strong alkali environment is necessary prepare high‐entropy layered (HELHs), which results uncontrollable structure, poor stability, scarce active sites. Here, universal synthesis of monolayer HELH frame mild presented, regardless product limit. Mild conditions allow this study precisely control fine structure composition final product. Consequently, surface area HELHs up 380.5 m 2 g −1 . The current density 100 mA cm −2 achieved 1 KOH at overpotential 259 mV, and, after 1000 h operation 20 , catalytic performance shows no obvious deterioration. engineering nanostructure open opportunities solve problems low intrinsic activity, very few sites, instability, conductance during OER LDH catalysts.

Language: Английский

Citations

62
Cation Substitution Induced d‐Band Center Modulation on Cobalt‐Based Spinel Oxides for Catalytic Ozonation DOI
Wei Qu,

Zhuoyun Tang,

Su Tang

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(44)

Published: July 4, 2023

Abstract Co 3 O 4 spinel is a promising transition metal oxide (TMO) catalyst for the catalytic ozonation of volatile organic compounds (VOCs). Herein, metal–organic frameworks (MOFs)‐derived Ni‐ and Mg‐ substituted catalysts retain similar structures, but display improved reduced performance methyl mercaptan (CH SH), respectively. Remarkably, NiCo 2 can still ≈90% removal CH SH after running 20 h at room temperature under an initial concentration 50 ppm 40 , relative humidity 60%, space velocity 300 000 mL −1 g exceeding reported values. Experimental characterizations have unveiled that substitution Ni Mg into altered surface acidity, oxygen species mobility, 2+ /Co 3+ ratio. The in situ Raman spectra reveal dynamic formation Co(III)‐O ad * via transformation atomic (O *) peroxide *). Theoretical calculations verify Ni‐substitution increases nonuniform charges Fermi density, leading to moderate increase d‐band center energy levels, thereby promoting specific adsorption/activation convert */O •OH/ 1 /•O − which contributes eliminate prevent poisoning. concept tuning provide valuable insights design other ozonation.

Language: Английский

Citations

58
Dual-site segmentally synergistic catalysis mechanism: boosting CoFeSx nanocluster for sustainable water oxidation DOI Creative Commons

Siran Xu,

Sihua Feng,

Yue Yu

et al.

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

Published: Feb. 26, 2024

Abstract Efficient oxygen evolution reaction electrocatalysts are essential for sustainable clean energy conversion. However, catalytic materials followed the conventional adsorbate mechanism (AEM) with inherent scaling relationship between key intermediates *OOH and *OH, or lattice-oxygen-mediated (LOM) possible lattice migration structural reconstruction, which not favorable to balance high activity stability. Herein, we propose an unconventional Co-Fe dual-site segmentally synergistic (DSSM) single-domain ferromagnetic catalyst CoFeS x nanoclusters on carbon nanotubes (CNT) (CFS-ACs/CNT), can effectively break without sacrificing Co 3+ (L.S, t 2g 6 e g 0 ) supplies strongest OH* adsorption energy, while Fe (M.S, 4 1 exposes strong O* adsorption. These dual-sites synergistically produce of Co-O-O-Fe intermediates, thereby accelerating release triplet-state ( ↑ O = ). As predicted, prepared CFS-ACs/CNT exhibits less overpotential than that commercial IrO 2 , as well approximately 633 h stability significant potential loss.

Language: Английский

Citations

58