Recent Advances of Electrocatalyst and Cell Design for Hydrogen Peroxide Production DOI Creative Commons
Xiao Huang, Min Young Song, Jingjing Zhang

et al.

Nano-Micro Letters, Journal Year: 2023, Volume and Issue: 15(1)

Published: April 7, 2023

Abstract Electrochemical synthesis of H 2 O via a selective two-electron oxygen reduction reaction has emerged as an attractive alternative to the current energy-consuming anthraquinone process. Herein, progress on electrocatalysts for generation, including noble metal, transition metal-based, and carbon-based materials, is summarized. At first, design strategies employed obtain with high electroactivity selectivity are highlighted. Then, critical roles geometry electrodes type reactor in striking balance boost rate systematically discussed. After that, potential strategy combine complementary properties catalysts optimal overall yield illustrated. Finally, remaining challenges promising opportunities high-efficient electrochemical production highlighted future studies.

Language: Английский

Iodide‐Induced Fragmentation of Polymerized Hydrophilic Carbon Nitride for High‐Performance Quasi‐Homogeneous Photocatalytic H2O2 Production DOI
Huinan Che, Xin Gao, Juan Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(48), P. 25546 - 25550

Published: Sept. 18, 2021

Polymeric carbon nitride (PCN) as a class of two-electron oxygen reduction reaction (2 e- ORR) photocatalyst has attracted much attention for H2 O2 production. However, the low activity and inferior selectivity 2 ORR greatly restrict production efficiency. Herein, we develop new strategy to synthesize hydrophilic, fragmented PCN by terminating polymerization (TP-PCN) effect iodide ions. The obtained TP-PCN with abundant edge active sites (AEASs), which can form quasi-homogeneous photocatalytic system, exhibits superior generation rate (3265.4 μM h-1 ), far surpassing other PCN-based photocatalysts. DFT calculations further indicate that is more favorable electron transiting from β spin-orbital π* orbitals , optimizes activation reduces energy barrier formation. This work provides concept designing functional photocatalysts understanding mechanism in

Language: Английский

Citations

406
Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide DOI
Shanyong Chen, Tao Luo, Kejun Chen

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(30), P. 16607 - 16614

Published: May 13, 2021

Abstract Electrochemical production of hydrogen peroxide (H 2 O ) through two‐electron (2 e − oxygen reduction reaction (ORR) is an on‐site and clean route. Oxygen‐doped carbon materials with high ORR activity H selectivity have been considered as the promising catalysts, however, there still a lack direct experimental evidence to identify true active sites at complex surface. Herein, we propose chemical titration strategy decipher oxygen‐doped nanosheet (OCNS 900 catalyst for ORR. The OCNS exhibits outstanding performances onset potential 0.825 V (vs. RHE), mass 14.5 A g −1 0.75 RHE) rate 770 mmol h in flow cell, surpassing most reported catalysts. Through selective C=O, C−OH, COOH groups, found that C=O species contributed electrocatalytic were ORR, which corroborated by theoretical calculations.

Language: Английский

Citations

245
Recent advances in strategies for highly selective electrocatalytic N2 reduction toward ambient NH3 synthesis DOI
Qian Liu, Tong Xu, Yonglan Luo

et al.

Current Opinion in Electrochemistry, Journal Year: 2021, Volume and Issue: 29, P. 100766 - 100766

Published: May 15, 2021

Language: Английский

Citations

229
Selective hydrogen peroxide conversion tailored by surface, interface, and device engineering DOI Creative Commons
Junying Tang, Tianshuo Zhao, Devan Solanki

et al.

Joule, Journal Year: 2021, Volume and Issue: 5(6), P. 1432 - 1461

Published: May 21, 2021

Language: Английский

Citations

178
Amorphous Boron Carbide on Titanium Dioxide Nanobelt Arrays for High‐Efficiency Electrocatalytic NO Reduction to NH3 DOI
Jie Liang, Pengyu Liu, Qinye Li

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(18)

Published: Feb. 25, 2022

Electrocatalytic NO reduction is regarded as an attractive strategy to degrade the contaminant into useful NH3 , but lack of efficient and stable electrocatalysts facilitate such multiple proton-coupled electron-transfer processes impedes its applications. Here, we report on developing amorphous B2.6 C supported a TiO2 nanoarray Ti plate (a-B2.6 C@TiO2 /Ti) -producing nanocatalyst with appreciable activity durability toward electroreduction. It shows yield 3678.6 μg h-1 cm-2 FE 87.6 %, superior /Ti (563.5 42.6 %) a-B2.6 C/Ti (2499.2 85.6 %). An /Ti-based Zn-NO battery achieves power density 1.7 mW 1125 . in-depth understanding catalytic mechanisms gained by theoretical calculations.

Language: Английский

Citations

173
Proximity Electronic Effect of Ni/Co Diatomic Sites for Synergistic Promotion of Electrocatalytic Oxygen Reduction and Hydrogen Evolution DOI
Min Li, Houyu Zhu, Qing Yuan

et al.

Advanced Functional Materials, Journal Year: 2022, Volume and Issue: 33(4)

Published: Nov. 13, 2022

Abstract The modulation effect manifests an encouraging potential to enhance the performance of single‐atom catalysts; however, in‐depth study about this for isolated diatomic sites (DASs) remains a great challenge. Herein, proximity electronic (PEE) Ni/Co DASs is proposed that anchored in N‐doped carbon (N‐C) substrate (NiCo DASs/N‐C) synergistic promoting electrocatalytic oxygen reduction reaction (ORR) and hydrogen evolution (HER). Benefiting from PEE adjacent Ni by four nitrogen (Ni‐N 4 ) moiety, NiCo DASs/N‐C catalyst exhibits superior ORR HER activity. In situ characterization results suggest Co (Co‐N as main active site O 2 adsorption‐activation process, which promotes formation key *OOH desorption *OH intermediate accelerate multielectron kinetics. Theoretical calculation reveals Ni‐N modulator can effectively adjust localization Co‐N site, *H adsorption on thereby boosting process significantly. This opens new opportunity rationally regulating catalytic centers well provides guidance designing high‐efficiency bifunctional electrocatalysts promising applications.

Language: Английский

Citations

171
A Pentagonal Defect-Rich Metal-Free Carbon Electrocatalyst for Boosting Acidic O2 Reduction to H2O2 Production DOI

Chang Zhang,

Wangqiang Shen, Kun Guo

et al.

Journal of the American Chemical Society, Journal Year: 2023, Volume and Issue: unknown

Published: May 9, 2023

Metal-free carbon-based materials are considered one of the most promising two-electron oxygen reduction reaction (2e– ORR) electrocatalysts for green synthesis hydrogen peroxide (H2O2). However, reported carbon perform much more effectively in alkalis than acids. Herein, by creatively using fullerene (C60) as precursor subject to ammonia treatment, we designed and synthesized a pentagonal defect-rich nitrogen-doped nanomaterial (PD/N–C). It achieves outstanding ORR activity, 2e– selectivity, stability acidic electrolytes, surpassing benchmark PtHg4 alloy catalyst. Impressively, flow cell based on PD/N–C catalyst nearly 100% Faraday efficiency with remarkable H2O2 yield, representing best improvement among all metal-free catalysts. Experimental theoretical results reveal that such superb performance originates from synergism between defects nitrogen dopants. This work presents an effective strategy design construction highly efficient acid-resistant production beyond.

Language: Английский

Citations

160
Conductive Two-Dimensional Magnesium Metal–Organic Frameworks for High-Efficiency O2 Electroreduction to H2O2 DOI
Kai Dong, Jie Liang, Yuanyuan Wang

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(10), P. 6092 - 6099

Published: May 6, 2022

Direct electrosynthesis of H2O2 via a two-electron oxygen reduction reaction (2e– ORR) under ambient conditions is emerging as promising solution toward on-site applications for the replacement energy-consuming, waste-intensive, and indirect anthraquinone process. To date, state-of-the-art 2e– ORR catalysis mostly performed with transition-metal-based materials, while main-group element-based catalysts are much less established, which there an urgent need proper understanding. Herein, we report conductive two-dimensionally layered Mg3(hexaiminotriphenylene)2 electrocatalyst selective hydrogenation O2 to synthesize (selectivity >90%) robust high catalytic efficiency. In situ spectroscopic monitoring reactions kinetic studies not only illustrate mechanisms on but confirm that Mg2+ center serving real active site responsible critical intermediate OOH* forming event. Additionally, in-depth density functional theory calculations further discuss excellent activity selectivity production.

Language: Английский

Citations

151
Magnetron sputtering enabled sustainable synthesis of nanomaterials for energy electrocatalysis DOI
Jie Liang, Qian Liu, Tingshuai Li

et al.

Green Chemistry, Journal Year: 2021, Volume and Issue: 23(8), P. 2834 - 2867

Published: Jan. 1, 2021

This review summarizes recent advances in developing sputtered nanomaterials as catalysts for energy electrocatalysis. In-depth insights into architecture/compositional design, synthesis, mechanism, and performance are provided.

Language: Английский

Citations

139
N-doped carbon nanotubes supported CoSe2 nanoparticles: A highly efficient and stable catalyst for H2O2 electrosynthesis in acidic media DOI Open Access
Longcheng Zhang, Jie Liang,

Luchao Yue

et al.

Nano Research, Journal Year: 2021, Volume and Issue: 15(1), P. 304 - 309

Published: April 26, 2021

Language: Английский

Citations

131