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

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

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

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

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Progress in metal-organic-framework-based single-atom catalysts for environmental remediation

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

Published: Oct. 4, 2022

Language: Английский

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Identification of Dynamic Active Sites Among Cu Species Derived from MOFs@CuPc for Electrocatalytic Nitrate Reduction Reaction to Ammonia

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

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

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

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Highly accessible atomically dispersed FeNx sites coupled with Fe3C@C core-shell nanoparticles boost the oxygen catalysis for ultra-stable rechargeable Zn-air batteries

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

Published: May 15, 2023

Language: Английский

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Flower-like Nanozyme with Highly Porous Carbon Matrix Induces Robust Oxidative Storm against Drug-Resistant Cancer

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

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Atomically Dispersed Iron Regulating Electronic Structure of Iron Atom Clusters for Electrocatalytic H₂O₂ Production and Biomass Upgrading

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

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Surface Engineered Single‐atom Systems for Energy Conversion

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

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

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

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