Recent advances in Fe‐N‐C single‐atom site coupled synergistic catalysts for boosting oxygen reduction reaction DOI Creative Commons
Katam Srinivas, Zhuo Chen,

Hesheng Yu

et al.

Electron, Journal Year: 2024, Volume and Issue: 2(1)

Published: Feb. 1, 2024

Abstract Metal–air batteries, fuel cells, and electrochemical H 2 O production currently attract substantial consideration in the energy sector owing to their efficiency eco‐consciousness. However, broader use is hindered by complex oxygen reduction reaction (ORR) that occurs at cathodes involves intricate electron transfers. Despite significant ORR performance of platinum‐based catalysts, high cost, operational limitations, susceptibility methanol poisoning hinder implementation. This emphasizes need for efficient non‐precious metal‐based electrocatalysts. A promising approach utilizing single‐atom catalysts (SACs) featuring metal–nitrogen–carbon (M‐N‐C) coordination sites. SACs offer advantages such as optimal utilization metal atoms, uniform active centers, precisely defined catalytic sites, robust metal–support interactions. symmetrical distribution around central atom a site (M‐N 4 ) often results suboptimal performance. challenge can be addressed carefully tailoring surrounding environment center. review specifically focuses on recent advancements Fe‐N within Fe‐N‐C SACs. It highlights strategy coupling sites with clusters and/or nanoparticles, which enhances intrinsic activity. By capitalizing interplay between associated species, overall improved. The combines findings from experimental studies density functional theory simulations, covering synthesis strategies coupled synergistic characterization techniques, influence particles offering comprehensive outlook, aims encourage research into high‐efficiency Fe real‐world applications coming years.

Language: Английский

Review of Carbon Support Coordination Environments for Single Metal Atom Electrocatalysts (SACS) DOI Creative Commons

Wanqing Song,

Caixia Xiao,

Jia Ding

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(1)

Published: April 20, 2023

This topical review focuses on the distinct role of carbon support coordination environment single-atom catalysts (SACs) for electrocatalysis. The article begins with an overview atomic configurations in SACs, including a discussion advanced characterization techniques and simulation used understanding active sites. A summary key electrocatalysis applications is then provided. These processes are oxygen reduction reaction (ORR), evolution (OER), hydrogen (HER), nitrogen (NRR), dioxide (CO

Language: Английский

Citations

139
Dual‐Sites Coordination Engineering of Single Atom Catalysts for Full‐Temperature Adaptive Flexible Ultralong‐Life Solid‐State Zn−Air Batteries DOI

Tengteng Gu,

Dantong Zhang,

Yan Yang

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(8)

Published: Dec. 14, 2022

Abstract High‐performance rechargeable Zn‐air batteries with long‐life stability are desirable for power applications in electric vehicles. The key component of the is bifunctional oxygen electrocatalyst, however, designing a electrocatalyst high intrinsic reversibility and durability challenge. Through density functional theory calculations, it found that catalytic activity originated from electronic geometric coordination structures synergistic effect Fe Co dual‐sites metal‐N 4 environment, assisting stronger hybridization orbitals between ( dxz, dz 2 ) OO* px, pz ), thus making O active ability site. These findings enable to development fancy dual single‐atom catalyst comprising adjacent FeN CoN sites on N‐doped carbon matrix (FeCo‐NC). FeCo‐NC exhibits extraordinary activities reduction evolution reaction (ORR/OER), which displays half‐wave potential (0.893 V) ORR, low overpotential (343 mV) at 10 mA cm −2 OER. assembled air‐electrode works well flexible solid‐state battery specific capacity 747.0 mAh g −1 , long‐time more than 400 h (30 °C), also superior performance extreme temperatures (−30 °C–60 °C).

Language: Английский

Citations

103
Progress in metal-organic-framework-based single-atom catalysts for environmental remediation DOI
Wei Qu, Cheng Chen,

Zhuoyun Tang

et al.

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 474, P. 214855 - 214855

Published: Oct. 4, 2022

Language: Английский

Citations

82
Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia DOI Creative Commons
Xue-Yang Ji, Ke Sun, Zhikun Liu

et al.

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: April 30, 2023

Direct electrochemical nitrate reduction reaction (NITRR) is a promising strategy to alleviate the unbalanced nitrogen cycle while achieving electrosynthesis of ammonia. However, restructuration high-activity Cu-based electrocatalysts in NITRR process has hindered identification dynamical active sites and in-depth investigation catalytic mechanism. Herein, Cu species (single-atom, clusters, nanoparticles) with tunable loading supported on N-doped TiO2/C are successfully manufactured MOFs@CuPc precursors via pre-anchor post-pyrolysis strategy. Restructuration behavior among co-dependent potential, as evidenced by advanced operando X-ray absorption spectroscopy, there exists an incompletely reversible transformation restructured structure initial state. Notably, CuN4&Cu4 deliver high NH3 yield 88.2 mmol h-1 gcata-1 FE (~ 94.3%) at - 0.75 V, resulting from optimal adsorption NO3- well rapid conversion *NH2OH *NH2 intermediates originated modulation charge distribution d-band center for site. This work not only uncovers have but also identifies dynamic that play critical role efficient electrocatalytic

Language: Английский

Citations

79
Single Cu–N4sites enable atomic Fe clusters with high-performance oxygen reduction reactions DOI

Shuwen Wu,

Shang Jiang,

Shaoqing Liu

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(8), P. 3576 - 3586

Published: Jan. 1, 2023

Atomic Fe clusters functionalized by Cu–N 4 sites with enhanced oxygen reduction reactions (ORRs) in alkaline and acidic media.

Language: Английский

Citations

63
Highly accessible atomically dispersed FeNx sites coupled with Fe3C@C core-shell nanoparticles boost the oxygen catalysis for ultra-stable rechargeable Zn-air batteries DOI
Katam Srinivas, Zhuo Chen, Fei Ma

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 335, P. 122887 - 122887

Published: May 15, 2023

Language: Английский

Citations

50
Flower-like Nanozyme with Highly Porous Carbon Matrix Induces Robust Oxidative Storm against Drug-Resistant Cancer DOI
Yuxin Xing, Lin Li, Yuhua Chen

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(7), P. 6731 - 6744

Published: March 22, 2023

Reactive oxygen species (ROS) generators are sparking breakthroughs in sensitization and treatment of therapy-resistant tumors, yet the efficacy is drastically compromised by limited substrate concentrations, short lifetimes free radicals, restricted oxidative damage. Herein, a flower-like nanozyme with highly permeable leaflets accommodating catalytic metal sites was developed to address challenges boosting product accessibility. In formation zeolite imidazole framework, cobalt ions promoted polymerization deposition polydopamine. The polymers acted as stiffener for preventing framework collapse maneuvering pore reopening during carbonization. single-atom/cluster porous matrix generated peroxidase/oxidase-like activities high efficiency (Kcat/Km) up 6 orders magnitude greater than that conventional nano-/biozymes. Thereby, robust ROS storm induced selective catalysis led rapid accumulation damage failure antioxidant antiapoptotic defense synchronization drug-resistant cancer cells. By synergy redox homeostasis disrupter co-delivered, significantly antitumor realized vivo. This work offers route kinetically favorable advancing tumors.

Language: Английский

Citations

49
Atomically Dispersed Iron Regulating Electronic Structure of Iron Atom Clusters for Electrocatalytic H2O2 Production and Biomass Upgrading DOI
Hui Xu, Shengbo Zhang, Xinyuan Zhang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(52)

Published: Nov. 10, 2023

The integration of highly active single atoms (SAs) and atom clusters (ACs) into an electrocatalyst is critically important for high-efficiency two-electron oxygen reduction reaction (2e- ORR) to hydrogen peroxide (H2 O2 ). Here we report a tandem impregnation-pyrolysis-etching strategy fabricate the oxygen-coordinated Fe SAs ACs anchored on bacterial cellulose-derived carbon (BCC) (FeSAs/ACs-BCC). As electrocatalyst, FeSAs/ACs-BCC exhibits superior electrocatalytic activity selectivity toward 2e- ORR, affording onset potential 0.78 V (vs. RHE) high H2 96.5 % in 0.1 M KOH. In flow cell reactor, also achieves production with yield rate 12.51±0.18 mol gcat-1 h-1 faradaic efficiency 89.4 %±1.3 at 150 mA cm-2 . Additionally, feasibility coupling produced electro-Fenton process valorization ethylene glycol was explored detail. theoretical calculations uncover that effectively regulate electronic structure which are ORR sites, resulting optimal binding strength *OOH intermediate production.

Language: Английский

Citations

48
Surface Engineered Single‐atom Systems for Energy Conversion DOI

Yutang Yu,

Zijian Zhu, Hongwei Huang

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(16)

Published: Jan. 10, 2024

Abstract Single‐atom catalysts (SACs) are demonstrated to show exceptional reactivity and selectivity in catalytic reactions by effectively utilizing metal species, making them a favorable choice among the different active materials for energy conversion. However, SACs still early stages of conversion, problems like agglomeration low conversion efficiency hampering their practical applications. Substantial research focus on support modifications, which vital SAC stability due intimate relationship between atoms support. In this review, category supports variety surface engineering strategies employed SA systems summarized, including site (heteroatom doping, vacancy introducing, groups grafting, coordination tunning) structure (size/morphology control, cocatalyst deposition, facet engineering, crystallinity control). Also, merits single‐atom systematically introduced. Highlights comprehensive summary discussions utilization surface‐engineered diversified applications photocatalysis, electrocatalysis, thermocatalysis, devices. At end potential obstacles using field discussed. This review aims guide rational design manipulation target‐specific capitalizing characteristic benefits engineering.

Language: Английский

Citations

31
Single-atom tailored atomically-precise nanoclusters for enhanced electrochemical reduction of CO2-to-CO activity DOI Creative Commons

Yi‐Man Wang,

Fang‐Qin Yan, Qian‐You Wang

et al.

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

Published: Feb. 28, 2024

Abstract The development of facile tailoring approach to adjust the intrinsic activity and stability atomically-precise metal nanoclusters catalysts is great interest but remians challenging. Herein, well-defined Au 8 modified by single-atom sites are rationally synthesized via a co-eletropolymerization strategy, in which uniformly dispersed nanocluster co-entrenched on poly-carbazole matrix. Systematic characterization theoretical modeling reveal that functionalizing single-atoms enable altering electronic structures clusters, amplifies their electrocatalytic reduction CO 2 ~18.07 fold compared isolated clusters. rearrangements structure not only strengthen adsorption key intermediates *COOH, also establish favorable reaction pathway for reaction. Moreover, this strategy fixing cross-linked polymer networks efficiently deduce performance deactivation caused agglomeration during catalytic process. This work contribute explore improvement

Language: Английский

Citations

30