A Simultaneous Modulation Strategy to Construct High Dense and Accessible Co‐N4 Sites for Promoting Oxygen Reduction Reaction in Zn–Air Battery DOI
Xuan Xie, Hui Peng,

Kanjun Sun

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: 34(32)

Published: April 25, 2024

Abstract Transition metal‐nitrogen‐carbon single‐atom catalysts (M─N─C SACs) exhibit outstanding catalytic activity for the oxygen reduction reaction (ORR). However, these still face dual challenges of low density and utilization active sites in practical applications. Hence, a simultaneous modulation strategy to construct high‐density accessible Co‐N 4 on nitrogen‐doped porous carbon (Co H SA/NC), is reported. As expected, optimized Co SA/NC catalyst exhibits superior ORR with half‐wave potential value 0.874 V, outperforming that benchmark Pt/C catalyst. Importantly, mass turnover frequency are 14.7 13.3 times higher than low‐density single atom L respectively. Structural characterization functional theory (DFT) reveal structure high dense synergistically improve performance, which induced redistribution d orbital, resulting z 2 orbital has enough electron interact OOH * specie, thereby facilitating kinetic process ORR. Moreover, SA/NC‐based Zn–Air Battery (ZAB) also showed excellent device including high‐power (191.7 mW cm −2 ), specific capacity, stability (250 h), significantly Pt/C‐based ZABs.

Language: Английский

Microenvironment Engineering of Single/Dual‐Atom Catalysts for Electrocatalytic Application DOI Open Access
Yun Gao, Baozhong Liu, Dingsheng Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(31)

Published: Feb. 23, 2023

Single/dual-metal atoms supported on carbon matrix can be modulated by coordination structure and neighboring active sites. Precisely designing the geometric electronic uncovering structure-property relationships of single/dual-metal confront with grand challenges. Herein, this review summarizes latest progress in microenvironment engineering single/dual-atom sites via a comprehensive comparison single-atom catalyst (SACs) dual-atom catalysts (DACs) term design principles, modulation strategy, theoretical understanding structure-performance correlations. Subsequently, recent advances several typical electrocatalysis process are discussed to get general reaction mechanisms finely-tuned SACs DACs. Finally, full-scaled summaries challenges prospects given for This will provide new inspiration development atomically dispersed electrocatalytic application.

Language: Английский

Citations

181
Carbon‐Based Electrocatalysts for Acidic Oxygen Reduction Reaction DOI Creative Commons

Pengbo Cui,

Linjie Zhao, Yongde Long

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(14)

Published: Jan. 16, 2023

Abstract Oxygen reduction reaction (ORR) is vital for clean and renewable energy technologies, which require no fossil fuel but catalysts. Platinum (Pt) the best‐known catalyst ORR. However, its high cost scarcity have severely hindered devices (e.g., cells) large‐scale applications. Recent breakthroughs in carbon‐based metal‐free electrochemical catalysts (C‐MFECs) show great potential earth‐abundant carbon materials as low‐cost electrocatalysts towards ORR acidic media. This article provides a focused, critical review on C‐MFECs media with an emphasis advances structure design synthesis, fundamental understanding of structure‐property relationship electrocatalytic mechanisms, their applications proton exchange membrane cells. Current challenges future perspectives this emerging field are also discussed.

Language: Английский

Citations

147
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

107
Altering the spin state of Fe-N-C through ligand field modulation of single-atom sites boosts the oxygen reduction reaction DOI

Dongping Xue,

Pengfei Yuan, Su Jiang

et al.

Nano Energy, Journal Year: 2022, Volume and Issue: 105, P. 108020 - 108020

Published: Nov. 21, 2022

Language: Английский

Citations

102
High‐Density Atomic Fe–N4/C in Tubular, Biomass‐Derived, Nitrogen‐Rich Porous Carbon as Air‐Electrodes for Flexible Zn–Air Batteries DOI
Chuanlai Jiao, Zian Xu, Jingze Shao

et al.

Advanced Functional Materials, Journal Year: 2023, Volume and Issue: 33(20)

Published: Feb. 22, 2023

Abstract Developing low‐cost single‐atom catalysts (SACs) with high‐density active sites for oxygen reduction/evolution reactions (ORR/OER) are desirable to promote the performance and application of metal–air batteries. Herein, Fe nanoparticles precisely regulated single atoms supported on waste biomass corn silk (CS) based porous carbon ORR OER. The distinct hierarchical structure hollow tube morphology critical boosting ORR/OER through exposing more accessible sites, providing facile electron conductivity, facilitating mass transfer reactant. Moreover, enhanced intrinsic activity is mainly ascribed high (4.3 wt.%) loading content in as‐synthesized catalyst.Moreover, ultra‐high N doping (10 can compensate insufficient OER conventional FeNC catalysts. When as‐prepared assembled as air‐electrodes flexible Zn–air batteries, they perform a peak power density 101 mW cm −2 , stable discharge–charge voltage gap 0.73 V >44 h, which shows great potential Zinc–air battery. This work provides an avenue transform renewable materials into bifunctional electrocatalysts structure.

Language: Английский

Citations

89
FeNC Oxygen Reduction Electrocatalyst with High Utilization Penta‐Coordinated Sites DOI Creative Commons
Jesús Barrio, Angus Pedersen, Saurav Ch. Sarma

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 35(14)

Published: Feb. 5, 2023

Atomic Fe in N-doped carbon (FeNC) electrocatalysts for oxygen (O2 ) reduction at the cathode of proton exchange membrane fuel cells are most promising alternative to platinum-group-metal catalysts. Despite recent progress on atomic FeNC O2 reduction, their controlled synthesis and stability practical applications remain challenging. A two-step approach has recently led significant advances terms Fe-loading mass activity; however, utilization remains low owing difficulty building scaffolds with sufficient porosity that electrochemically exposes active sites. Herein, this issue is addressed by coordinating a highly porous nitrogen-doped support (≈3295 m2 g-1 ), prepared pyrolysis inexpensive 2,4,6-triaminopyrimidine Mg2+ salt site template porogen. Upon coordination, high electrochemical density 2.54 × 1019 sites gFeNC-1 record 52% FeNx based situ nitrite stripping achieved. The single atoms characterized pre- post-electrochemical accelerated stress testing aberration-corrected high-angle annular dark field scanning transmission electron microscopy, showing no clustering. Moreover, ex X-ray absorption spectroscopy low-temperature Mössbauer suggest presence penta-coordinated sites, which further studied functional theory calculations.

Language: Английский

Citations

83
A general approach to 3D-printed single-atom catalysts DOI
Fangxi Xie, Xiaolin Cui, Xing Zhi

et al.

Nature Synthesis, Journal Year: 2023, Volume and Issue: 2(2), P. 129 - 139

Published: Jan. 2, 2023

Language: Английский

Citations

81
Terbium-induced cobalt valence-band narrowing boosts electrocatalytic oxygen reduction DOI

Xuan Wang,

Juan Zhang, Pu Wang

et al.

Energy & Environmental Science, Journal Year: 2023, Volume and Issue: 16(11), P. 5500 - 5512

Published: Jan. 1, 2023

Tb 2 O 3 endows Co 3d with a narrow band and appropriate location via 3d–O 2p–Tb 4f gradient orbital coupling to efficiently enhance the oxygen reduction reaction.

Language: Английский

Citations

81
Advances and challenges of methanol-tolerant oxygen reduction reaction electrocatalysts for the direct methanol fuel cell DOI
Muhammad Aizaz Ud Din, Muhammad Idrees, Sidra Jamil

et al.

Journal of Energy Chemistry, Journal Year: 2022, Volume and Issue: 77, P. 499 - 513

Published: Nov. 23, 2022

Language: Английский

Citations

77
State-of-the-art single-atom catalysts in electrocatalysis: From fundamentals to applications DOI
Muhammad Humayun, Muhammad Israr, Abbas Khan

et al.

Nano Energy, Journal Year: 2023, Volume and Issue: 113, P. 108570 - 108570

Published: May 29, 2023

Language: Английский

Citations

59