Single‐Atomic Co‐N‐C Sites Anchored on Helical Carbonaceous Nanotubes for the Oxygen Reduction Reaction DOI Open Access

Jieling Zhang,

Yonghong Mou,

Weiran Suo

et al.

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

Published: Nov. 7, 2024

Abstract Metal‐coordinated N‐doped carbon (M‐N‐C) materials with highly curved structures have become a promising class of electrocatalysts for the oxygen reduction reaction (ORR). However, stability these remains problem due to traditional post‐metal loading strategy. Herein, single‐atomic Co‐N‐C active sites anchored on helical carbonaceous nanotubes (HCNTs) are prepared (Co‐N‐C@HCNT) by pyrolyzing Co porphyrins and polypyrroles (PPys) mixtures at high‐temperature one‐step method. Aberration‐corrected high‐angle annular dark‐field scanning transmission electron microscopy (HAADF‐STEM) X‐ray absorption fine structure (XAFS) measurements confirm Co‐N 4 coordination Co‐N‐C@HCNT. The optimized Co‐N‐C@HCNT exhibits excellent catalytic ORR activity half‐wave potential ( E 1/2 ) 0.86 V versus reversible hydrogen electrode (vs RHE) compared Co‐N‐C@CNT without = 0.81 vs measured in 0.1 m KOH. also displays slight current decrease (4%) after running 10 h featuring tightly HCNTs electrostatic interactions between metal PPys. Theoretical calculations indicate that can increase charge d‐band center site, which enhances electrocatalytic activity. This work provides simple but effective strategy construct M‐N‐C materials.

Language: Английский

Bifunctional Single Atom Catalysts for Rechargeable Zinc–Air Batteries: From Dynamic Mechanism to Rational Design DOI

Peng Zhang,

Kuo Chen, Jiaye Li

et al.

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

Published: June 7, 2023

Ever-growing demands for rechargeable zinc-air batteries (ZABs) call efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high utilization, structural tunability, and remarkable activity. Rational design SACs relies heavily on an in-depth understanding reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in mechanisms replace current trial error modes. Herein, fundamental oxygen reduction is first presented combining situ and/or operando characterizations theoretical calculations. By highlighting structure-performance relationships, rational regulation strategies are particularly proposed facilitate SACs. Furthermore, future perspectives challenges discussed. review provides thorough SACs, which expected pave avenue exploring optimum effective ZABs.

Language: Английский

Citations

101
Co(CN)3 catalysts with well-defined coordination structure for the oxygen reduction reaction DOI
Kai Sun, Juncai Dong, Hao Sun

et al.

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(12), P. 1164 - 1173

Published: Nov. 16, 2023

Language: Английский

Citations

77
Atomic-level polarization in electric fields of defects for electrocatalysis DOI Creative Commons
Jie Xu, Xiong‐Xiong Xue, Gonglei Shao

et al.

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

Published: Nov. 29, 2023

The thriving field of atomic defect engineering towards advanced electrocatalysis relies on the critical role electric polarization at scale. While this is proposed theoretically, spatial configuration, orientation, and correlation with specific catalytic properties materials are yet to be understood. Here, by targeting monolayer MoS2 rich in defects, we pioneer direct visualization such defects combining electron microscopy differential phase contrast technology. It revealed that asymmetric charge distribution caused facilitates adsorption H*, which originally activates sites for hydrogen evolution reaction (HER). Then, it has been experimentally proven atomic-level fields can enhance HER activity. This work bridges long-existing gap between directly revealing angstrom-scale correlating as-tuned materials; methodology here could also inspire future studies focusing mechanism understanding structure-property-performance relationship.

Language: Английский

Citations

45
Single‐Atom Iron Catalyst as an Advanced Redox Mediator for Anodic Oxidation of Organic Electrosynthesis DOI

Xin‐Yu Wang,

Yong‐Zhou Pan,

Jiarui Yang

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(27)

Published: April 23, 2024

Homogeneous electrocatalysts can indirect oxidate the high overpotential substrates through single-electron transfer on electrode surface, enabling efficient operation of organic electrosynthesis catalytic cycles. However, problems this chemistry still exist such as dosage, difficult recovery, and low efficiency. Single-atom catalysts (SACs) exhibit atom utilization excellent activity, hold great promise in addressing limitations homogeneous catalysts. In view this, we have employed Fe-SA@NC an advanced redox mediator to try change situation. was synthesized using encapsulation-pyrolysis method, it demonstrated remarkable performance a range reported reactions, construction various C-C/C-X bonds. Moreover, potential exploring new synthetic method for electrosynthesis. We develop electro-oxidative ring-opening transformation cyclopropyl amides. reaction system, showed good tolerance drug molecules with complex structures, well flow electrochemical syntheses gram-scale transformations. This work highlights SACs electrosynthesis, thereby opening avenue chemistry.

Language: Английский

Citations

28
Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization DOI Creative Commons
Yizhe Li, Yajie Li, Hao Sun

et al.

Nano-Micro Letters, Journal Year: 2024, Volume and Issue: 16(1)

Published: Feb. 29, 2024

Abstract The exploration of sustainable energy utilization requires the implementation advanced electrochemical devices for efficient conversion and storage, which are enabled by usage cost-effective, high-performance electrocatalysts. Currently, heterogeneous atomically dispersed catalysts considered as potential candidates a wide range applications. Compared to conventional catalysts, metal atoms in carbon-based have more unsaturated coordination sites, quantum size effect, strong metal–support interactions, resulting exceptional catalytic activity. Of these, dual-atomic (DACs) attracted extensive attention due additional synergistic effect between two adjacent atoms. DACs advantages full active site exposure, high selectivity, theoretical 100% atom utilization, ability break scaling relationship adsorption free on sites. In this review, we summarize recent research advancement DACs, includes (1) comprehensive understanding synergy atomic pairs; (2) synthesis DACs; (3) characterization methods, especially aberration-corrected scanning transmission electron microscopy synchrotron spectroscopy; (4) energy-related last part focuses great catalysis small molecules, such oxygen reduction reaction, CO 2 hydrogen evolution N reaction. future challenges opportunities also raised prospective section.

Language: Английский

Citations

25
Encaging Co nanoparticle in atomic Co N4-dispersed graphite nanopocket evokes high oxygen reduction activity for flexible Zn-air battery DOI

Yuandong Yang,

Yi Xiao, Linjie Zhang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2024, Volume and Issue: 347, P. 123792 - 123792

Published: April 24, 2024

Language: Английский

Citations

22
Asymmetric Coordination Regulating D‐Orbital Spin‐Electron Filling in Single‐Atom Iron Catalyst for Efficient Oxygen Reduction DOI
Yizhe Li, Hao Sun,

Longtao Ren

et al.

Angewandte Chemie International Edition, Journal Year: 2024, Volume and Issue: 63(28)

Published: May 9, 2024

The single-atom Fe-N-C catalyst has shown great promise for the oxygen reduction reaction (ORR), yet intrinsic activity is not satisfactory. There a pressing need to gain deeper understanding of charge configuration and develop rational modulation strategies. Herein, we have prepared Fe with co-coordination N O (denoted as Fe-N/O-C) adjacent defect, proposing strategy optimize d-orbital spin-electron filling sites by fine-tuning first coordination shell. Fe-N/O-C exhibits significantly better ORR compared its counterpart commercial Pt/C, much more positive half-wave potential (0.927 V) higher kinetic current density. Moreover, using catalyst, Zn-air battery proton exchange membrane fuel cell achieve peak power densities up 490 1179 mW cm

Language: Английский

Citations

22
Atomically dispersed multi-site catalysts: bifunctional oxygen electrocatalysts boost flexible zinc–air battery performance DOI
Shengchen Wang, Mengyang Zhang,

Xueqin Mu

et al.

Energy & Environmental Science, Journal Year: 2024, Volume and Issue: 17(14), P. 4847 - 4870

Published: Jan. 1, 2024

Based on the advancements in atomically dispersed multi-site catalysts for FZABs, this review discusses design methodologies to regulate performance of bifunctional oxygen electrocatalysts from electronic and geometric structures.

Language: Английский

Citations

21
Hetero‐Diatomic CoN4‐NiN4 Site Pairs with Long‐Range Coupling as Efficient Bifunctional Catalyst for Rechargeable Zn–Air Batteries DOI Creative Commons

Yue Yang,

Bin Li,

Yining Liang

et al.

Advanced Science, Journal Year: 2024, Volume and Issue: 11(22)

Published: March 30, 2024

Abstract In this study, Co/Ni‐NC catalyst with hetero‐diatomic Co/Ni active sites dispersed on nitrogen‐doped carbon matrix is synthesized via the controlled pyrolysis of ZIF‐8 containing Co 2+ and Ni compounds. Experimental characterizations theoretical calculations reveal that are atomically uniformly in pairs CoN 4 ‐NiN an intersite distance ≈0.41 nm, there long‐range d – coupling between more electron delocalization for higher bifunctional activity. Besides, situ grown nanotubes at edges particles allow high electronic conductivity electrocatalysis process. Electrochemical evaluations demonstrate superior ORR OER bifunctionality a narrow potential gap only 0.691 V long‐term durability, significantly prevailing over single‐atom Co‐NC Ni‐NC catalysts benchmark Pt/C RuO 2 catalysts. catalyzed Zn–air batteries achieve specific capacity 771 mAh g −1 long continuous operation period up to 340 h small voltage ≈0.65 V, also much Pt/C‐RuO .

Language: Английский

Citations

18
Machine learning-assisted dual-atom sites design with interpretable descriptors unifying electrocatalytic reactions DOI Creative Commons
Xiaoyun Lin, Xiaowei Du, Shican Wu

et al.

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

Published: Sept. 17, 2024

Low-cost, efficient catalyst high-throughput screening is crucial for future renewable energy technology. Interpretable machine learning a powerful method accelerating design by extracting physical meaning but faces huge challenges. This paper describes an interpretable descriptor model to unify activity and selectivity prediction multiple electrocatalytic reactions (i.e., O

Language: Английский

Citations

17