High-density asymmetric iron dual-atom sites for efficient and stable electrochemical water oxidation DOI Creative Commons
Lili Zhang,

Ning Zhang,

Huishan Shang

et al.

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

Published: Nov. 1, 2024

Double-atom catalysts (DACs) have opened distinctive paradigms in the field of rapidly developing atomic catalysis owing to their great potential for promoting catalytic performance various reaction systems. However, increasing loading and extending service life metal active centres represents a considerable challenge efficient utilization DACs. Here, we rationally design asymmetric nitrogen, sulfur-coordinated diatomic iron on highly defective nitrogen-doped carbon nanosheets (denoted A-Fe

Language: Английский

Multifunctional carbon nitride nanoarchitectures for catalysis DOI
Prashant Kumar, Gurwinder Singh, Xinwei Guan

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7602 - 7664

Published: Jan. 1, 2023

Carbon nitrides, with feasibility of tailored band gap via suitable nanoarchitectonics, are deemed as best catalysts amongst existing materials, especially for HER, OWS, COR, NRR, water oxidation, pollutant removal, and organocatalysis.

Language: Английский

Citations

95
Atomically dispersed Ni activates adjacent Ce sites for enhanced electrocatalytic oxygen evolution activity DOI Creative Commons
Zhihao Pei, Huabin Zhang, Zhi‐Peng Wu

et al.

Science Advances, Journal Year: 2023, Volume and Issue: 9(26)

Published: June 28, 2023

Manipulating the intrinsic activity of heterogeneous catalysts at atomic level is an effective strategy to improve electrocatalytic performances but remains challenging. Here, atomically dispersed Ni anchored on CeO2 particles entrenched peanut-shaped hollow nitrogen-doped carbon structures (a-Ni/CeO2@NC) rationally designed and synthesized. The as-prepared a-Ni/CeO2@NC catalyst exhibits substantially boosted greatly reduced overpotential for oxygen evolution reaction. Experimental theoretical results demonstrate that decoration isolated species over induces electronic coupling redistribution, thus resulting in activation adjacent Ce sites around atoms accelerated kinetics. This work provides a promising explore regulation improvement level, thereby improving activity.

Language: Английский

Citations

87
The Heterointerface between Fe1/NC and Selenides Boosts Reversible Oxygen Electrocatalysis DOI

Huanran Zheng,

Shibin Wang, Shoujie Liu

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(40)

Published: June 13, 2023

Abstract The rational design and construction of efficient inexpensive bifunctional oxygen electrocatalysts are highly desirable for the development rechargeable Zn–air batteries (ZABs). Although single‐atom Fe sites anchored on N‐doped carbon catalysts (Fe 1 /NC) ensure high reduction reaction activity, their unitary atomically dispersed active center faces difficult condition in catalyzing evolution simultaneously. Herein, a composite catalyst containing heterointerface between /NC selenides ((Fe,Co)Se 2 ) is constructed. obtained (Fe,Co)Se @Fe exhibits extremely narrow potential gap 0.616 V remarkable stability alkaline media, outperforming benchmark (Pt/C+RuO : 0.720 V). Experimental results density functional theory calculations reveal that accelerates electron transfer provides more moderate adsorption sites, which endow with catalytic activity. This study not only superior ZABs, but also enriches application multifunctional energy storage conversion devices.

Language: Английский

Citations

71
Structural engineering of atomic catalysts for electrocatalysis DOI Creative Commons

Tianmi Tang,

Xue Bai, Zhenlü Wang

et al.

Chemical Science, Journal Year: 2024, Volume and Issue: 15(14), P. 5082 - 5112

Published: Jan. 1, 2024

This review systematically introduces how to regulate the electronic structure and geometric configuration of atomic catalysts achieve high-efficiency electrocatalysis performances by analyzing detailed electrocatalytic applications mechanisms.

Language: Английский

Citations

62
Potential Dominates Structural Recombination of Single Atom Mn Sites for Promoting Oxygen Reduction Reaction DOI

Miaomiao Tong,

Fanfei Sun,

Gengyu Xing

et al.

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

Published: Nov. 13, 2023

Single atom sites (SAS) often undergo structural recombination in oxygen reduction reaction (ORR), while the effect of valence state and reconstruction on active centers needs to be investigated thoroughly. Herein, Mn-SAS catalyst with uniform precise Mn-N4 configuration is rationally designed. We utilize operando synchrotron radiation track dynamic evolution during ORR. Under applied potential, into Mn-N3 C further Mn-N2 C2 configurations clarified. Simultaneously, states Mn are increased from +3.0 +3.8 then decreased +3.2. When potential removed, returned its initial Mn+3.0 -N4 configuration. Such successive evolutions optimize electronic geometric structures as evidenced by theory calculations. The evolved Mn+3.8 -N3 Mn+3.2 -N2 respectively adjust O2 adsorption reduce energy barrier rate-determining step. Thus, it can achieve an onset 0.99 V, superior stability over 10,000 cycles, a high turnover frequency 1.59 s-1 at 0.85 VRHE. Our present work provides new insights construction well-defined SAS catalysts regulating centers.

Language: Английский

Citations

57
Nanoconfinement steers nonradical pathway transition in single atom fenton-like catalysis for improving oxidant utilization DOI Creative Commons
Yan Meng,

Yu-Qin Liu,

Chao Wang

et al.

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

Published: June 22, 2024

Abstract The introduction of single-atom catalysts (SACs) into Fenton-like oxidation promises ultrafast water pollutant elimination, but the limited access to pollutants and oxidant by surface catalytic sites intensive consumption still severely restrict decontamination performance. While nanoconfinement SACs allows drastically enhanced reaction kinetics, detailed regulatory mechanisms remain elusive. Here, we unveil that, apart from local enrichment reactants, pathway shift is also an important cause for reactivity enhancement nanoconfined SACs. electronic structure cobalt site altered confining it within nanopores mesostructured silica particles, which triggers a fundamental transition singlet oxygen electron transfer 4-chlorophenol oxidation. changed accelerated interfacial mass render system up 34.7-fold higher degradation rate raised peroxymonosulfate utilization efficiency (from 61.8% 96.6%) relative unconfined control. It demonstrates superior other electron-rich phenolic compounds, good environment robustness, high stability treating real lake water. Our findings deepen knowledge catalysis may inspire innovations in low-carbon purification technologies heterogeneous applications.

Language: Английский

Citations

50
Design yolk-shelled FeCo layered double hydroxide via a “one-stone-two-birds” strategy for oxygen evolution reaction DOI

Dongyu Han,

Lin Hao,

Rou Wang

et al.

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 336, P. 126363 - 126363

Published: Jan. 11, 2024

Language: Английский

Citations

41
Atomic Engineering of 3D Self‐Supported Bifunctional Oxygen Electrodes for Rechargeable Zinc‐Air Batteries and Fuel Cell Applications DOI
Milan Babu Poudel, Mannix P. Balanay, Prakash Chandra Lohani

et al.

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: 14(30)

Published: May 28, 2024

Abstract The oxygen evolution reaction (OER) and reduction (ORR) are cornerstone half reactions involved in many renewable energy technologies. High‐density single‐atom catalysts maximize the atom utilization isolated active sites. Furthermore, introduction of pyri‐N into carbon‐based nanostructures as an electrocatalyst creates abundance Here, innovative strategy is reported based on atomic scale dispersion Co atoms enriched carbon nanotube encapsulated Ni nanoparticles grown 3D electrospun nanofiber nano‐assemblies. Notably, SA Ni‐NCNT/CNF exhibited excellent OER ORR activity terms low overpotentials higher half‐wave potentials. atomically distributed allows maximum exposure sites dominated multidimensional skeleton, synergistic effects with greatly reduced delocalization around metal centers provided ideal environment for interactions intermediates, thus facilitating 4e − pathway, evidenced by DFT calculations. Moreover, Zn‐air batteries using a air cathode high‐power density admirable specific capacity. This studies may provide avenue rational modulation cost‐effective, large‐scale synthesis bifunctional electrocatalysts rechargeable anion exchange membrane fuel cell.

Language: Английский

Citations

37
Defect Engineering for Enhanced Electrocatalytic Oxygen Reaction on Transition Metal Oxides: The Role of Metal Defects DOI
Jingxuan Zheng, Dapeng Meng, Junxin Guo

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(28)

Published: April 26, 2024

Metal defect engineering is a highly effective strategy for addressing the prevalent high overpotential issues associated with transition metal oxides functioning as dual-function commercial oxygen reduction reaction/oxygen evolution reaction catalysts increasing their activity and stability. However, formation energy of defects poses challenge to development strategies precisely control selectivity during formation. Here, density functional theory calculations are used demonstrate that altering pathway releases atoms chlorides, which effectively reduces defects. The on monometallic oxide surface (Mn, Fe, Co, Ni) selectively produced using chlorine plasma. characterization reveal catalytic enhanced owing electronic delocalization induced by defects, theoretical overpotential. Notably, ab initio molecular dynamics calculations, ex situ XPS, in ATR-SEIRAS suggest improve adsorption reactive species active sites enhance efficiency product desorption, thereby boosting performance.

Language: Английский

Citations

33
Emerging Strategies for the Synthesis of Correlated Single Atom Catalysts DOI
Yucong Huang, Jingjing Xiong, Zhigang Zou

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Feb. 9, 2024

Abstract People have been looking for an energy‐efficient and sustainable method to produce future chemicals decades. Heterogeneous single‐atom catalysts (SACs) with atomic dispersion of robust, well‐characterized active centers are highly desirable. In particular, correlated SACs cooperative interaction between adjacent single atoms allow the switching single‐site pathway dual or multisite pathway, thus promoting bimolecular more complex reactions synthesis fine chemicals. Herein, structural uniqueness SACs, including intermetal distance electronic in homo/heteronuclear metal sites is featured. Recent advances production methods showcasing research status challenges traditional (such as pyrolysis, wet impregnation, confined synthesis) building a comprehensive multimetallic SAC library, summarized. Emerging strategies such process automation continuous‐flow highlighted, minimizing inconsistency laboratory batch allowing high throughput screening upscaling toward next‐stage chemical by SACs.

Language: Английский

Citations

31