Dual‐Active‐Sites Single‐Atom Catalysts for Advanced Applications DOI
Shaolong Zhang,

Minchen Hou,

Yanliang Zhai

et al.

Small, Journal Year: 2023, Volume and Issue: 19(42)

Published: June 15, 2023

Abstract Dual‐Active‐Sites Single‐Atom catalysts (DASs SACs) are not only the improvement of SACs but also expansion dual‐atom catalysts. The DASs contains dual active sites, one which is a single atomic site, and other site can be atom or type endowing with excellent catalytic performance wide range applications. categorized into seven types, including neighboring mono metallic SACs, bonded non‐bonded bridged asymmetric metal nonmetal combined space separated SACs. Based on above classification, general methods for preparation comprehensively described, especially their structural characteristics discussed in detail. Meanwhile, in‐depth assessments variety applications electrocatalysis, thermocatalysis photocatalysis provided, as well unique mechanism addressed. Moreover, prospects challenges related highlighted. authors believe great expectations this review will provide novel conceptual methodological perspectives exciting opportunities further development application

Language: Английский

Neodymium‐Evoked Valence Electronic Modulation to Balance Reversible Oxygen Electrocatalysis DOI

Chuang Fan,

Xuan Wang,

Xiangrui Wu

et al.

Advanced Energy Materials, Journal Year: 2022, Volume and Issue: 13(2)

Published: Nov. 23, 2022

Abstract Suffering from the competition adsorption between oxygen reduction reaction (ORR) and evolution (OER), development of high‐efficiency electrocatalysts with bifunctional properties still remains a challenge. Herein, novel effective neodymium‐evoked valence electronic perturbation strategy to improve balance reversible electrocatalysis metallic cobalt sites is proposed. To heighten coupling Nd Co, metal‐organic‐framework‐induced method chosen prepare target catalyst atomic Nd‐doped Co on an N‐doped carbon substrate. The as‐prepared presents excellent electrocatalytic low overpotential 288 mV at 10 mA cm −2 for OER high half‐wave potential 0.85 V ORR. robust stabilities both ORR are also proven. electrochemical in situ Raman spectra confirm surface dynamic change transformation intermediates by noting formation Co–OOH. Theoretical calculations verify that balanced owing strong 3d‐Nd 4f orbital effect below Fermi level. Moreover, practicability further demonstrated solid‐state rechargeable Zn‐Air batteries, which exhibit large power density long cycling life.

Language: Английский

Citations

142
Hierarchically Porous Carbons with Highly Curved Surfaces for Hosting Single Metal FeN4 Sites as Outstanding Oxygen Reduction Catalysts DOI Creative Commons
Guangbo Chen, Ruihu Lu, Chenzhao Li

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(32)

Published: May 3, 2023

Iron-nitrogen-carbon (FeNC) materials have emerged as a promising alternative to platinum-group metals for catalyzing the oxygen reduction reaction (ORR) in proton-exchange-membrane fuel cells. However, their low intrinsic activity and stability are major impediments. Herein, an FeN-C electrocatalyst with dense FeN4 sites on hierarchically porous carbons highly curved surfaces (denoted -hcC) is reported. The -hcC catalyst displays exceptional ORR acidic media, high half-wave potential of 0.85 V (versus reversible hydrogen electrode) 0.5 m H2 SO4 . When integrated into membrane electrode assembly, corresponding cathode maximum peak power density 0.592 W cm-2 demonstrates operating durability over 30 000 cycles under harsh /air conditions, outperforming previously reported Fe-NC electrocatalysts. These experimental theoretical studies suggest that carbon support fine-tunes local coordination environment, lowers energies Fe d-band centers, inhibits adsorption oxygenated species, which can enhance stability. This work provides new insight nanostructure-activity correlation catalysis. It also offers approach designing advanced single-metal-site catalysts energy-conversion applications.

Language: Английский

Citations

105
Recent Progress of Diatomic Catalysts: General Design Fundamentals and Diversified Catalytic Applications DOI

Yifan Hu,

Zesheng Li, Bolin Li

et al.

Small, Journal Year: 2022, Volume and Issue: 18(46)

Published: Sept. 23, 2022

Abstract In recent years, some experiments and theoretical work have pointed out that diatomic catalysts not only retain the advantages of monoatomic catalysts, but also introduce a variety interactions, which exceed limit catalytic performance can be applied to many fields. Here, interaction between adjacent metal atoms in is elaborated: synergistic effect, spacing enhancement effect (geometric effect), electronic effect. With regard classification characterization various new are classified into four categories: heteronuclear/homonuclear, with/without carbon carriers, their measures introduced explained detail. aspect preparation widely used atomic layer deposition method, metal–organic framework derivative simple ball milling method introduced, with emphasis on formation mechanism catalysts. Finally, effective control strategies key applications electrocatalysis, photocatalysis, thermal catalysis, other fields given.

Language: Английский

Citations

90
Core–Shell Carbon‐Based Bifunctional Electrocatalysts Derived from COF@MOF Hybrid for Advanced Rechargeable Zn–Air Batteries DOI
Wei Li,

Jingyun Wang,

Junxiang Chen

et al.

Small, Journal Year: 2022, Volume and Issue: 18(31)

Published: July 9, 2022

The development of highly active carbon-based bifunctional electrocatalysts for both the oxygen evolution reaction (OER) and reduction (ORR) is desired, but still full challenges in rechargeable Zn-air batteries. Metal organic frameworks (MOFs) covalent (COFs) have gained great attention various applications due to their attractive features structural tunability, high surface area porosity. Herein, a core-shell structured hybrid electrocatalyst (H-NSC@Co/NSC), which contains density sites MOF-derived shell (Co/NSC) COF-derived hollow core (H-NSC), successfully fabricated by direct pyrolysis covalently-connected COF@ZIF-67 hybrid. H-NSC@Co/NSC manifests excellent catalytic properties toward OER ORR with small potential gap (∆E = 0.75 V). assembled battery exhibits power-density 204.3 mW cm-2 stable rechargeability, outperforming that Pt/C+RuO2 battery. Density functional theory calculations reveal electronic structure carbon on Co/NSC can be effectively modulated embedded Co nanoparticles (NPs), facilitating adsorption intermediates leading enhanced activity. This work will provide strategy design highly-efficient application energy conversion storage.

Language: Английский

Citations

77
Nanoarchitectonics of Hollow Covalent Organic Frameworks: Synthesis and Applications DOI
Lijin Huang, Juan Yang, Yusuke Asakura

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(10), P. 8918 - 8934

Published: May 2, 2023

Hollow covalent organic frameworks (COFs) have gained significant attention because of their specific properties, including enhanced surface-to-volume ratio, large surface area, hierarchical structure, highly ordered nanostructures, and excellent chemical stability. These intrinsic characteristics endow hollow COFs with fascinating physicochemical properties make them attractive for widespread applications, such as catalysis, energy storage, drug delivery, therapy, sensing, environmental remediation. This review focuses on the recent developments in synthesis derivatives. In addition, practical applications various fields are summarized. Finally, challenges future opportunities terms synthetic methodologies discussed. expected to play an important role materials science.

Language: Английский

Citations

76
Fe, Cu dual-metal single atom catalyst on commercial carbon black for efficient oxygen reduction reaction DOI

Hongzhou Yang,

He Huang,

Qing Wang

et al.

Journal of Materials Chemistry A, Journal Year: 2023, Volume and Issue: 11(12), P. 6191 - 6197

Published: Jan. 1, 2023

Fe, Cu dual metal single atom catalyst on commercial carbon black exhibited excellent oxygen reduction reaction performance.

Language: Английский

Citations

62
Highly active, ultra-low loading single-atom iron catalysts for catalytic transfer hydrogenation DOI Creative Commons

Zhidong An,

Piaoping Yang,

Delong Duan

et al.

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Oct. 20, 2023

Highly effective and selective noble metal-free catalysts attract significant attention. Here, a single-atom iron catalyst is fabricated by saturated adsorption of trace onto zeolitic imidazolate framework-8 (ZIF-8) followed pyrolysis. Its performance toward catalytic transfer hydrogenation furfural comparable to state-of-the-art up four orders higher than other Fe catalysts. Isotopic labeling experiments demonstrate an intermolecular hydride mechanism. First principles simulations, spectroscopic calculations experiments, kinetic correlations reveal that the synthesis creates pyrrolic Fe(II)-plN3 as active center whose flexibility manifested being pulled out plane, enabled defects, crucial for collocating reagents allowing chemistry proceed. The catalyzes chemoselectively several substrates possesses unique trait whereby hindered more acidic hydrogen donors. This work paves way noble-metal free important chemical reactions.

Language: Английский

Citations

58
Optimization Strategies of Covalent Organic Frameworks and Their Derivatives for Electrocatalytic Applications DOI
Liyuan Xiao, Zhenlü Wang, Jingqi Guan

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 34(11)

Published: Nov. 27, 2023

Abstract Covalent organic frameworks (COFs) are crystalline porous polymers that can be precisely integrated by building blocks to achieve pre‐designed composition, components, and functions, making them a powerful platform for the development of molecular devices in field electrocatalysis. The precise control channel/dopant positions highly ordered network structures COFs provide an ideal material system applications advanced In this paper, topological structure design synthesis methods reviewed detail, their principles deeply analyzed. addition, derivatives electrocatalysis systematically summarized optimization strategies proposed. Finally, application prospects challenges may encountered future prospected, providing helpful guidance research.

Language: Английский

Citations

55
Pyridinic Nitrogen Sites Dominated Coordinative Engineering of Subnanometric Pd Clusters for Efficient Alkynes’ Semihydrogenation DOI
Rui Zhang, Zhilin Liu,

Shaohang Zheng

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(11)

Published: Jan. 3, 2023

Supported metal catalysts have played an important role in optimizing selective semihydrogenation of alkynes for fine chemicals. There into, nitrogen-doped carbons, as a type promising support materials, attracted extensive attentions. However, due to the general phenomenon random doping nitrogen species support, it is still atremendous challenge finely identify which configuration dominates catalytic property alkynes' semihydrogenation. Herein, reported that uniform mesoporous N-doped carbon spheres derived from polypyrrole are used supports immobilized subnanometric Pd clusters, provide particular platform research influence configurations on Comprehensive experimental results and density functional theory calculation indicate pyridinic behavior clusters. The high contents sites offer abundant coordination sites, greatly reduces energy barrier rate-determining reaction step makes clusters own activity. electron effect between highly selective. Additionally, good mesostructures also promote fast transport substrate. Based above, catalyst Pd@PPy-600 exhibits activity (99%) selectivity (96%) phenylacetylene (C8 H6 )

Language: Английский

Citations

52
Metal-organic framework-based materials as key components in electrocatalytic oxidation and reduction reactions DOI

Soheila Sanati,

Ali Morsali, Hermenegildo Garcı́a

et al.

Journal of Energy Chemistry, Journal Year: 2023, Volume and Issue: 87, P. 540 - 567

Published: Sept. 6, 2023

Language: Английский

Citations

51