Manipulating Metal Cations Microenvironment for Highly Selective Electrochemical Water Oxidation to Hydrogen Peroxide DOI

Lanke Luo,

Mingxuan Li,

Haohai Dong

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 15(1), P. 193 - 200

Published: Dec. 16, 2024

Electrochemical two-electron water oxidation (2e– WOR) represents a promising approach for the renewable and on-site production of H2O2, potentially replacing anthraquinone process. Nevertheless, it faces intense competition from conventional four-electron oxygen evolution reaction (OER), resulting in low selectivity, high overpotential, yield. Herein, taking carbon-based structures with 2e– WOR selectivity as model catalysts, by manipulating electrolyte, increased maximum Faraday efficiency H2O2 to 71 ± 3%, an rate 11.7 μmol cm–2 min–1. The activity was found be most sensitive alkali metal cations following order: Cs+ > K+ Na+ Li+. In situ spectroscopy characterization confirmed that larger facilitate generation peroxide species; this is because, on one hand, can regulate electronic catalyst sites improve adsorption intermediates; other cation-hydrogen interaction regulates stable coordination cation, realizes reforming hydrogen bond network, prevents its further into O2. With help flow electro-synthetic cell, we successfully achieve rapid degradation organic pollutants preparation solid (sodium peroxycarbonate). This work not only enriches understanding cationic mechanisms but also provides implications rational optimization strategies electrode/electrolyte interface.

Language: Английский

Methods and Prospects for Enhancing Heterogeneous Fenton Catalytic Activity DOI Open Access
Qian Wang, Liangliang Wang, Junxia Wang

et al.

ChemistrySelect, Journal Year: 2025, Volume and Issue: 10(1)

Published: Jan. 1, 2025

Abstract As an advanced oxidation process that can efficiently remove organic pollutants in water, Fenton has attracted much attention recent years. Compared to homogeneous Fenton, it a wider applicability, wide pH range, higher degradation efficiency, lower environmental impact, and treatment cost. However, the heterogeneous reaction also some limitations, such as deactivation of catalyst, rate being limited by solid–liquid interface mass transfer. Therefore, development efficient stable catalytic system is focus research at present. In this paper, catalysis are introduced, construction characteristics mechanism iron base, copper transition metals their oxides, chelating agents, carbon materials, supported catalysts, photocatalysis systematically summarized. addition, strategies for formation Fe II promotion H 2 O decomposition were discussed, pathway catalyst matter summarized order provide technical support further on catalysts.

Language: Английский

Citations

1
Highly Efficient Metal-Free Coal-Based Carbon Aerogel Catalyst for Oxygen Reduction to Produce Hydrogen Peroxide DOI

Lingman Xia,

Mingsheng Luo,

Changke Shao

et al.

Industrial & Engineering Chemistry Research, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 10, 2025

In this study, a highly efficient metal-free catalyst derived supported on coal-based carbon aerogel was successfully synthesized for the two-electron transfer oxygen reduction reaction (2e– ORR) to produce hydrogen peroxide (H2O2). The catalyst, with its high specific surface area and hierarchical porous structure, demonstrated exceptional selectivity H2O2 under alkaline conditions. By optimization of synthesis drying conditions, particularly through use supercritical technology, physicochemical properties were significantly enhanced. Notably, gel obtained CO2 exhibited superior over 1311 m2·g–1. 95% at potential 0.5 V vs SHE using material from study. It also revealed that attributed layered edge active sites, which are rich in carbonyl (C=O) carboxyl (COOH) groups. situ FTIR Raman spectroscopic analyses confirmed two-electron-transfer ORR mechanism

Language: Английский

Citations

0
Modulating Electronic Spin State of Perovskite Fluoride by Ni─F─Mn Bond Activating the Dynamic Site of Oxygen Reduction Reaction DOI Open Access
Shuang Yang,

Jiaqin Chen,

Rong Li

et al.

Small, Journal Year: 2025, Volume and Issue: unknown

Published: Jan. 23, 2025

Abstract Establishing the relationship between catalytic performance and material structure is crucial for developing design principles highly active catalysts. Herein, a type of perovskite fluoride, NH 4 MnF 3 , which owns strong‐field coordination including fluorine ammonia, in situ grown on carbon nanotubes (CNTs) used as model to study improve intrinsic activity through heteroatom doping strategies. This approach optimizes spin‐dependent orbital interactions alter charge transfer catalyst reactants. As result, oxygen reduction reaction (ORR) CNTs significantly enhanced by partial substitution Mn sites with Ni, such half‐wave potential (E 1/2 ) 0.86 V limiting current density 5.26 mA cm −2 are comparable those commercial Pt/C Experimental theoretical calculations reveal that introduction Ni promotes lattice distortion, adjusts electronic states centers, facilitates transition from low‐spin intermediate‐spin states, shifts d ‐band center closer Fermi level. establishes novel designing high‐performance perovskite‐based fluoride electrocatalysts modulating spin states.

Language: Английский

Citations

0
P-block cathode electrocatalysts: A critical review of their role and impact on oxygen reduction reaction in fuel cells applications DOI

Siti Haziyah Mohd Chachuli,

Sharifah Najiha Timmiati, Kee Shyuan Loh

et al.

Journal of Industrial and Engineering Chemistry, Journal Year: 2025, Volume and Issue: unknown

Published: Feb. 1, 2025

Language: Английский

Citations

0
A review of two electrons oxygen reduction reaction fundamentals to produce hydrogen peroxide over various cobalt-based electrocatalysts DOI
Karimi Haqmal Ahmad Samir,

Zahidi Niaz Mohammad,

Danishyar Abdul Sattar

et al.

Materials Research Innovations, Journal Year: 2025, Volume and Issue: unknown, P. 1 - 13

Published: Feb. 26, 2025

Language: Английский

Citations

0
Dual‐Functional Catalyst of Amorphous TiO2 Embedded in Mesoporous Carbon Hollow Spheres for H2O2 Electrosynthesis DOI Open Access
Zhaohui Wang, Kun Li, Junling Hu

et al.

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 12, 2025

Abstract H 2 O production in coupled electrochemical systems, where is generated through 2e‐pathway of water oxidation (2e‐WOR) at anode and oxygen reduction (2e‐ORR) cathode, offers an advanced alternative to the anthraquinone process. However, efficiency such system often hindered by limited activity selectivity electrocatalysts. Herein, a dual‐functional catalyst composed amorphous TiO embedded mesoporous carbon hollow spheres (TiO x @MCHS) reported, which exhibits exceptional electrocatalytic performance for both 2e‐WOR 2e‐ORR. By employing @MCHS‐loaded electrodes as cathode membrane‐free flow cell with 4 м K CO 3 /KHCO electrolyte, rate 108.3 µmol min −1 cm −2 Faradaic (FE) ≈145% are achieved voltage ≈2.5 V under constant current 240 mA (anode: 1 , cathode: ). Experimental computational results reveal crucial role low‐coordinated Ti optimizing adsorption intermediates involved two electrode reaction pathways, thereby enhancing these processes. This work establishes new paradigm development electrocatalysts design novel coupled‐electrolysis enabling scalable sustainable electrosynthesis.

Language: Английский

Citations

0
Synergistic Zn-Cd Bimetallic Engineering in ZIFs for High-Chloride 2e− ORR to H2O2 in Simulated Neutral Seawater DOI Open Access
Xu Wang, Nan Wang, Kunpeng Liu

et al.

Materials, Journal Year: 2025, Volume and Issue: 18(8), P. 1786 - 1786

Published: April 14, 2025

Marine biofouling causes significant economic losses, and conventional antifouling methods are often associated with environmental pollution. Hydrogen peroxide (H2O2), as a clean energy source, has gained increasing attention in recent years. Meanwhile, electrocatalytic 2e− oxygen reduction reaction (ORR) for H2O2 production received growing interest. However, the majority of current studies conducted on acidic or alkaline electrolytes, research ORR neutral NaCl solutions remains rare. Here, bimetallic Zn-Cd zeolitic imidazolate framework (ZnCd-ZIF) is rationally designed to achieve chloride-resistant catalysis under simulated seawater conditions (pH 7.5, 3.5% Cl−). Experimental results demonstrate that ZnCd-ZIF catalyst exhibits an exceptional selectivity 70% at 0.3 VRHE, surpassing monometallic Zn-ZIF (60%) Cd-ZIF (50%). Notably, reaches 120 mmol g−1 Cl−-containing electrolyte, exhibiting strong resistance structural corrosion Cl− poisoning. This work not only pioneers effective strategy designing catalysts adapted marine environments but also advances practical implementation seawater-based electrochemical synthesis.

Language: Английский

Citations

0
Reconstructed Hydroxyl Coordination Field Enhances Mass Transfer for Efficient Electrocatalytic Water Oxidation DOI
Haomin Jiang,

Haohai Dong,

Yicheng Liu

et al.

Small, Journal Year: 2024, Volume and Issue: 21(6)

Published: Dec. 29, 2024

Abstract Mass transfer factor plays an indispensable role in high current density to accelerate the oxygen evolution reaction (OER) process, yet research on modulating reactant mass transport remains limited. Herein, by leveraging dual acid‐base properties of aluminum sites, both activation electronic activity layer for layered double hydroxides (LDH) and construction interlayer hydroxide coordination field (IHCF) have been achieved through situ electrochemical reconstruction. It not only facilitates charge surface catalytic transformation intermediates but, most notably, presence IHCF significantly enhances reactants. As a result, overpotential LDHs with is 164 mV, better than reported Ni‐based catalysts. Deuterium kinetic isotope effect experiments pH‐dependence measurements demonstrate that effectively substrate capability structural stability, thereby accelerating proton‐coupled electron process. To further validate characteristics, stability tests alkaline flow electrolyzer show catalysts maintain over 1000 h at density. This work suggests can be utilized design synthesis efficient water oxidation practical application.

Language: Английский

Citations

1
Manipulating Metal Cations Microenvironment for Highly Selective Electrochemical Water Oxidation to Hydrogen Peroxide DOI

Lanke Luo,

Mingxuan Li,

Haohai Dong

et al.

ACS Catalysis, Journal Year: 2024, Volume and Issue: 15(1), P. 193 - 200

Published: Dec. 16, 2024

Electrochemical two-electron water oxidation (2e– WOR) represents a promising approach for the renewable and on-site production of H2O2, potentially replacing anthraquinone process. Nevertheless, it faces intense competition from conventional four-electron oxygen evolution reaction (OER), resulting in low selectivity, high overpotential, yield. Herein, taking carbon-based structures with 2e– WOR selectivity as model catalysts, by manipulating electrolyte, increased maximum Faraday efficiency H2O2 to 71 ± 3%, an rate 11.7 μmol cm–2 min–1. The activity was found be most sensitive alkali metal cations following order: Cs+ > K+ Na+ Li+. In situ spectroscopy characterization confirmed that larger facilitate generation peroxide species; this is because, on one hand, can regulate electronic catalyst sites improve adsorption intermediates; other cation-hydrogen interaction regulates stable coordination cation, realizes reforming hydrogen bond network, prevents its further into O2. With help flow electro-synthetic cell, we successfully achieve rapid degradation organic pollutants preparation solid (sodium peroxycarbonate). This work not only enriches understanding cationic mechanisms but also provides implications rational optimization strategies electrode/electrolyte interface.

Language: Английский

Citations

0