Sb2S3-templated synthesis of sulfur-doped Sb-N-C with hierarchical architecture and high metal loading for H2O2 electrosynthesis DOI Creative Commons

Minmin Yan,

Zengxi Wei, Zhichao Gong

et al.

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

Published: Jan. 23, 2023

Abstract Selective two-electron (2e − ) oxygen reduction reaction (ORR) offers great opportunities for hydrogen peroxide (H 2 O electrosynthesis and its widespread employment depends on identifying cost-effective catalysts with high activity selectivity. Main-group metal nitrogen coordinated carbons (M-N-Cs) are promising but remain largely underexplored due to the low metal-atom density lack of understanding in structure-property correlation. Here, we report using a nanoarchitectured Sb S 3 template synthesize high-density (10.32 wt%) antimony (Sb) single atoms nitrogen- sulfur-codoped carbon nanofibers (Sb-NSCF), which exhibits both selectivity (97.2%) mass (114.9 A g −1 at 0.65 V) toward 2e ORR alkaline electrolyte. Further, when evaluated practical flow cell, Sb-NSCF shows production rate 7.46 mol catalyst h negligible loss 75-h continuous electrolysis. Density functional theory calculations demonstrate that coordination configuration dopants synergistically contribute enhanced Sb-N 4 moieties.

Language: Английский

P and Cu Dual Sites on Graphitic Carbon Nitride for Photocatalytic CO2Reduction to Hydrocarbon Fuels with High C2H6Evolution DOI
Gang Wang, Zhe Chen, Tao Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(40)

Published: Aug. 15, 2022

The light-driven CO2 reduction to multi-carbon products is especially meaningful, while the low efficiency of multi-electron transfer and sluggish C-C coupling greatly hinder its development. Herein, we report a photocatalyst comprising P Cu dual sites anchored on graphitic carbon nitride (P/Cu SAs@CN), which achieves high C2 H6 evolution rate 616.6 μmol g-1 h-1 in reducing hydrocarbons. detailed spectroscopic characterizations identify formation charge-enriched sites, where isolated atoms serve as hole capture during photocatalysis. Theoretical simulations combined with situ FTIR measurement reveal kinetically feasible process for intermediate (*OC-COH) confirm favorable production P/Cu SAs@CN photocatalyst. This work offers new insights into design atomic precision toward highly efficient photocatalytic conversion value-added products.

Language: Английский

Citations

225
Long‐Range Interactions in Diatomic Catalysts Boosting Electrocatalysis DOI
Wenhao Li, Jiarui Yang, Dingsheng Wang

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(52)

Published: Oct. 6, 2022

Abstract The simultaneous presence of two active metal centres in diatomic catalysts (DACs) leads to the occurrence specific interactions between sites. Such interactions, referred as long‐range (LRIs), play an important role determining rate and selectivity a reaction. optimal combination must be determined achieve targeted efficiency. To date, various types DACs have been synthesised applied electrochemistry. However, LRIs not systematically summarised. Herein, regulation, mechanism, electrocatalytic applications are comprehensively summarised discussed. In addition basic information above, challenges, opportunities, future development proposed order present overall view reference for research.

Language: Английский

Citations

214
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
Coordination Symmetry Breaking of Single‐Atom Catalysts for Robust and Efficient Nitrate Electroreduction to Ammonia DOI
Xue‐Feng Cheng, Jinghui He, Haoqing Ji

et al.

Advanced Materials, Journal Year: 2022, Volume and Issue: 34(36)

Published: July 16, 2022

Nitrate electrocatalytic reduction (NO3 RR) for ammonia production is a promising strategy to close the N-cycle from nitration contamination, as well an alternative Haber-Bosch process with less energy consumption and carbon dioxide release. However, current long-term stability of NO3 RR catalysts usually tens hours, far requirements industrialization. Here, symmetry-broken Cusingle-atom are designed, catalytic activity retained after operation more than 2000 h, while average rate 27.84 mg h-1 cm-2 at industrial level density 366 mA achieved, obtaining good balance between stability. Coordination symmetry breaking achieved by embedding one Cu atom in graphene nanosheets two N O atoms cis-configuration, effectively lowering coordination symmetry, rendering active site polar, accumulating NO3- near electrocatalyst surface. Additionally, cis-coordination splits 3d orbitals, which generates orbital-symmetry-matched π-complex key intermediate *ONH reduces barrier, compared σ-complex generated other catalysts. These results reveal critical role single-atom catalysts, prompting design coordination-symmetry-broken electrocatalysts toward possible

Language: Английский

Citations

212
Synergistic Fe−Se Atom Pairs as Bifunctional Oxygen Electrocatalysts Boost Low‐Temperature Rechargeable Zn‐Air Battery DOI
Yao Wang, Jiao Wu, Shuaihao Tang

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Feb. 18, 2023

Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe-Se atom pairs supported on N-doped carbon (Fe-Se/NC). The obtained Fe-Se/NC shows a noteworthy oxygen catalytic performance with low potential difference of 0.698 V, far superior to that reported Fe-based single-atom catalysts. theoretical calculations reveal p-d orbital hybridization around the leads remarkably asymmetrical polarized charge distributions. based solid-state rechargeable Zn-air batteries (ZABs-Fe-Se/NC) present stable charge/discharge 200 h (1090 cycles) at 20 mA cm-2 25 °C, which is 6.9 times ZABs-Pt/C+Ir/C. At extremely temperature -40 ZABs-Fe-Se/NC displays an ultra-robust cycling 741 (4041 1 , about 11.7 More importantly, could be operated for 133 (725 even 5 °C.

Language: Английский

Citations

206
Dual‐Atom Support Boosts Nickel‐Catalyzed Urea Electrooxidation DOI
Xiaobo Zheng, Jiarui Yang, Peng Li

et al.

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(22)

Published: March 24, 2023

Nickel-based catalysts have been regarded as one of the most promising electrocatalysts for urea oxidation reaction (UOR), however, their activity is largely limited by inevitable self-oxidation Ni species (NSOR) during UOR. Here, we proposed an interface chemistry modulation strategy to trigger occurrence UOR before NSOR via constructing a 2D/2D heterostructure that consists ultrathin NiO anchored Ru-Co dual-atom support (Ru-Co DAS/NiO). Operando spectroscopic characterizations confirm this unique triggering mechanism on surface DAS/NiO. Consequently, fabricated catalyst exhibits outstanding with low potential 1.288 V at 10 mA cm-2 and remarkable long-term durability more than 330 h operation. DFT calculations demonstrate favorable electronic structure induced heterointerface endows energetically NSOR.

Language: Английский

Citations

202
Lattice Strain and Schottky Junction Dual Regulation Boosts Ultrafine Ruthenium Nanoparticles Anchored on a N-Modified Carbon Catalyst for H2 Production DOI

Zhuoli Jiang,

Shaojia Song, Xiaobo Zheng

et al.

Journal of the American Chemical Society, Journal Year: 2022, Volume and Issue: 144(42), P. 19619 - 19626

Published: Oct. 12, 2022

Ruthenium-based materials are considered great promising candidates to replace Pt-based catalysts for hydrogen production in alkaline conditions. Herein, we adopt a facile method rationally design neoteric Schottky catalyst which uniform ultrafine ruthenium nanoparticles featuring lattice compressive stress supported on nitrogen-modified carbon nanosheets (Ru NPs/NC) efficient evolution reaction (HER). Lattice strain and junction dual regulation ensures that the Ru NPs/NC with an appropriate nitrogen content displays superb H2 media. Particularly, NPs/NC-900 1.3% attractive activity durability HER low overpotential of 19 mV at 10 mA cm-2 1.0 M KOH electrolyte. The situ X-ray absorption fine structure measurements indicate low-valence nanoparticle shrinking Ru-Ru bond acts as catalytic active site during process. Furthermore, multiple spectroscopy analysis density functional theory calculations demonstrate tunes electron adsorption center, thus enhancing activity. This strategy provides novel concept advanced electrocatalysts production.

Language: Английский

Citations

201
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

187
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
Carbon Nitride Photocatalysts with Integrated Oxidation and Reduction Atomic Active Centers for Improved CO2Conversion DOI
Honghui Ou, Shangbo Ning, Peng Zhu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(34)

Published: June 18, 2022

Single-atom active-site catalysts have attracted significant attention in the field of photocatalytic CO2 conversion. However, designing active sites for reduction and H2 O oxidation simultaneously on a photocatalyst combining corresponding half-reaction system is still difficult. Here, we synthesized bimetallic single-atom with two compatible centers Mn Co carbon nitride (Mn1 Co1 /CN). Our experimental results density functional theory calculations showed that center promotes by accumulating photogenerated holes. In addition, activation increasing bond length angle molecules. Benefiting from synergistic effect atomic centers, Mn1 /CN exhibited CO production rate 47 μmol g-1 h-1 , which significantly higher than single-metal photocatalyst.

Language: Английский

Citations

171