Efficient Proton-exchange Membrane Fuel Cell Performance of Atomic Fe Sites via p–d Hybridization with Al Dopants DOI
Yarong Liu, Jiaxin Li,

Zunhang Lv

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(18), P. 12636 - 12644

Published: April 27, 2024

Orbital hybridization to regulate the electronic structures and surface chemisorption properties of transition metals is great importance for boosting oxygen reduction reaction (ORR) in proton-exchange membrane fuel cells (PEMFCs). Herein, we developed a core–shell rambutan-like nanocarbon catalyst (FeAl-RNC) with atomically dispersed Fe–Al atom pairs from metal–organic framework (MOF) material. Experimental theoretical results demonstrate that strong p–d orbital between Al Fe an asymmetric electron distribution moderate adsorption strength intermediates, rendering enhanced intrinsic ORR activity. Additionally, structure FeAl-RNC abundant micropores macropores can enhance density active sites, stability, transport pathways PEMFC. The FeAl-RNC-based PEMFC achieves excellent activity (68.4 mA cm–2 at 0.9 V), high peak power (1.05 W cm–2), good stability only 7% current loss after 100 h 0.7 V under H2–O2 condition.

Language: Английский

Atomically dispersed materials: Ideal catalysts in atomic era DOI
Tao Gan, Dingsheng Wang

Nano Research, Journal Year: 2023, Volume and Issue: 17(1), P. 18 - 38

Published: May 25, 2023

Language: Английский

Citations

214
Sustainable zinc–air battery chemistry: advances, challenges and prospects DOI
Qichen Wang, Shubham Kaushik, Xin Xiao

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(17), P. 6139 - 6190

Published: Jan. 1, 2023

Sustainable zinc-air batteries (ZABs) are considered promising energy storage devices owing to their inherent safety, high density, wide operating temperature window, environmental friendliness, etc., showing great prospect for future large-scale applications. Thus, tremendous efforts have been devoted addressing the critical challenges associated with sustainable ZABs, aiming significantly improve efficiency and prolong operation lifespan. The growing interest in ZABs requires in-depth research on oxygen electrocatalysts, electrolytes, Zn anodes, which not systematically reviewed date. In this review, fundamentals of electrocatalysts air cathodes, physicochemical properties ZAB issues strategies stabilization anodes summarized from perspective fundamental characteristics design principles. Meanwhile, significant advances situ/operando characterization highlighted provide insights into reaction mechanism dynamic evolution electrolyte|electrode interface. Finally, several thoughts perspectives provided regarding opportunities ZABs. Therefore, review provides a thorough understanding advanced chemistry, hoping that timely comprehensive can shed light upcoming horizons prosperous area.

Language: Английский

Citations

190
The reformation of catalyst: From a trial-and-error synthesis to rational design DOI
Ligang Wang, Jiabin Wu,

Shunwu Wang

et al.

Nano Research, Journal Year: 2023, Volume and Issue: 17(4), P. 3261 - 3301

Published: Sept. 27, 2023

Language: Английский

Citations

183
Nanoscale Metal Particle Modified Single‐Atom Catalyst: Synthesis, Characterization, and Application DOI Open Access
Runze Chen, Shenghua Chen, Liqiang Wang

et al.

Advanced Materials, Journal Year: 2023, Volume and Issue: 36(2)

Published: July 13, 2023

Single-atom catalysts (SACs) have attracted considerable attention in heterogeneous catalysis because of their well-defined active sites, maximum atomic utilization efficiency, and unique unsaturated coordinated structures. However, effectiveness is limited to reactions requiring sites containing multiple metal atoms. Furthermore, the loading amounts single-atom must be restricted prevent aggregation, which can adversely affect catalytic performance despite high activity individual The introduction nanoscale particles (NMPs) into SACs (NMP-SACs) has proven an efficient approach for improving performance. A comprehensive review urgently needed systematically introduce synthesis, characterization, application NMP-SACs mechanisms behind superior This first presents classifies different through NMPs enhance SACs. It then summarizes currently reported synthetic strategies state-of-the-art characterization techniques NMP-SACs. Moreover, electro/thermo/photocatalysis, reasons are discussed. Finally, challenges perspectives future design advanced addressed.

Language: Английский

Citations

110
Tailoring Oxygen Reduction Reaction Kinetics of Fe−N−C Catalyst via Spin Manipulation for Efficient Zinc–Air Batteries DOI
Huiwen Zhang, Hsiao‐Chien Chen,

Solmaz Feizpoor

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: 36(25)

Published: April 9, 2024

The interaction between oxygen species and metal sites of various orbitals exhibits intimate correlation with the reduction reaction (ORR) kinetics. Herein, a new approach for boosting inherent ORR activity atomically dispersed Fe-N-C matrix is represented by implanting Fe atomic clusters nearby. as-prepared catalyst delivers excellent half-wave potentials 0.78 0.90 V in acidic alkaline solutions, respectively. decent can also be validated from high-performance rechargeable Zn-air battery. experiments density functional theory calculations reveal that electron spin-state monodispersed active transferred low spin (LS, t

Language: Английский

Citations

106
Ampere-Level Nitrate Electroreduction to Ammonia over Monodispersed Bi-Doped FeS2 DOI
Guike Zhang, Guohui Wang,

Yuying Wan

et al.

ACS Nano, Journal Year: 2023, Volume and Issue: 17(21), P. 21328 - 21336

Published: Oct. 23, 2023

Electrochemical conversion of NO3– into NH3 (NO3RR) holds an enormous prospect to simultaneously yield valuable and alleviate pollution. Herein, we report monodispersed Bi-doped FeS2 (Bi–FeS2) as a highly effective NO3RR catalyst. Atomic coordination characterizations Bi–FeS2 disclose that the isolated Bi dopant coordinates with its adjacent Fe atom create unconventional p–d hybridized Bi–Fe dinuclear sites. Operando spectroscopic measurements combined theoretical calculations sites can synergistically enhance hydrogenation energetics NO3–-to-NH3 pathway, while suppressing competitive hydrogen evolution, leading high selectivity activity. Consequently, specially designed flow cell equipped exhibits rate 83.7 mg h–1 cm–2 near-100% Faradaic efficiency at ampere-level current density 1023.2 mA cm–2, together excellent long-term stability for 100 h electrolysis, ranking almost highest performance among all reported catalysts.

Language: Английский

Citations

97
Elucidation of the mechanistic origin of spin-state-dependent P-doped Fe single-atom catalysts for the oxidation of organic pollutants through peroxymonosulfate activation DOI
Yandong Chai,

Hongling Dai,

Xiaoguang Duan

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 341, P. 123289 - 123289

Published: Sept. 14, 2023

Language: Английский

Citations

93
A Janus dual-atom catalyst for electrocatalytic oxygen reduction and evolution DOI
Bing Tang, Yanan Zhou, Qianqian Ji

et al.

Nature Synthesis, Journal Year: 2024, Volume and Issue: 3(7), P. 878 - 890

Published: June 3, 2024

Language: Английский

Citations

92
A Fe Single Atom Seed‐Mediated Strategy Toward Fe3C/FeNC Catalysts with Outstanding Bifunctional ORR/OER Activities DOI Creative Commons

Jiangwei Chang,

Qi Zhang,

Jingkun Yu

et al.

Advanced Science, Journal Year: 2023, Volume and Issue: 10(22)

Published: May 31, 2023

The discovery of low-cost and high-performance bifunctional oxygen electrocatalysts is vital to the future commercialization rechargeable zinc-air batteries (ZABs). Herein, a Fe single atom seed-mediated strategy reported for fabrication Fe3 C species closely surrounded by FeN4 C active sites with strong electronic interactions built between them more importantly, creating optimized coordination environment, via subtly adjusting their ratio, favorable adsorption energies intermediates formed during reduction reaction (ORR) evolution (OER). Concretely, voltage difference (ΔE) ORR half-wave OER potential at current density 10 mA cm-2 compositionally-optimized FeNC/Fe3 C-op electrocatalyst only 0.668 V, endowing itself one best OER/ORR benchmarks. As demo, ZABs assembled as air cathode deliver remarkable specific capacity (818.1 mAh gZn-1 ) power (1013.9 mWh ), along excellent long-term durability (>450 h). This work extends methodology modulate activity atomic site, undoubtedly inspiring wide explorations on precise design electrocatalysts.

Language: Английский

Citations

91
Polystyrene Waste Thermochemical Hydrogenation to Ethylbenzene by a N-Bridged Co, Ni Dual-Atom Catalyst DOI
Runze Li, Zedong Zhang, Liang Xiao

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: 145(29), P. 16218 - 16227

Published: July 12, 2023

Recycling waste plastics requires the degradation of into small molecules. However, various products are widely distributed using traditional methods depolymerizing polystyrene (PS) such as catalytic pyrolysis and hydrogenolysis. Here, we creatively report a N-bridged Co, Ni dual-atom (Co-N-Ni) catalyst for targeted conversion PS to ethylbenzene via pressurized tandem fixed-bed reactor where hydropyrolysis is coupled with downstream vapor-phase hydrotreatment. The Co-N-Ni achieves 95 wt % 92 yield, significantly superior corresponding single-atom catalysts, enables real plastics. Theoretical calculations experimental results demonstrate that d-band center metal atoms well regulated in catalyst. Co site activates C═C bond more easily, while spatially optimizes adsorption configuration styrene molecule due electronic interaction. This also shows excellent durability provides new direction plastic degradation.

Language: Английский

Citations

85