Cd Single Atom as an Electron Mediator in an S‐Scheme Heterojunction for Artificial Photosynthesis of H₂O₂

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

Published: Feb. 13, 2025

Abstract Developing conductor‐mediated S‐scheme heterojunction photocatalysts imitating natural photosynthetic systems emerges as a promising approach to hydrogen peroxide (H 2 O ) production. However, achieving precise coupling between two semiconductors with charge shuttle and modulating the interfacial interactions still remain significant bottleneck. Herein, we propose catalyst architecture Cd single atom mediated formed by interfacing CdS TiO nanoparticles. This exhibits an H production rate high 60.33 µmol g −1 min under UV–vis light irradiation, which is attributed efficient transport at interface of thanks S‐scheme. In‐situ X‐ray photoelectron spectroscopy (XPS) electron spin resonance (ESR) spin‐trapping tests confirm transfer route. Femtosecond transient absorption (fs‐TA) other ex‐situ characterizations further corroborate across interface. work offers new perspective on constructing atoms heterojunctions enhance photocatalytic performance.

Language: Английский

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Recent Progress in Oxygen Reduction Reaction Toward Hydrogen Peroxide Electrosynthesis and Cooperative Coupling of Anodic Reactions

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

Published: March 13, 2025

Abstract Electrosynthesis of hydrogen peroxide (H 2 O ) via two‐electron oxygen reduction reaction (2e − ORR) is a promising alternative to the anthraquinone oxidation process. To improve overall energy efficiency and economic viability this catalytic process, one pathway develop advanced catalysts decrease overpotential at cathode, other couple 2e ORR with certain anodic reactions full cell voltage while producing valuable chemicals on both electrodes. The performance catalyst depends not only material itself but also environmental factors. Developing electrocatalysts high selectivity activity prerequisite for efficient H electrosynthesis, coupling appropriate would further enhance efficiency. Considering this, here comprehensive review presented latest progress state‐of‐the‐art in different media, microenvironmental modulation mechanisms beyond design, as well electrocatalytic system various reactions. This presents new insights regarding existing challenges opportunities within rapidly advancing field, along viewpoints future development electrosynthesis construction green roadmaps.

Language: Английский

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Electrocatalytic H2O2 production paired with value-added chemicals synthesis, contaminant remediation, and electricity generation

Chemical Engineering Journal, Journal Year: 2025, Volume and Issue: unknown, P. 159828 - 159828

Published: Jan. 1, 2025

Language: Английский

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A bimetallic CuFe layered double hydroxide supported on carbon black: An efficient and sustainable electrocatalyst for the electrochemical detection of Ornidazole

Journal of environmental chemical engineering, Journal Year: 2025, Volume and Issue: unknown, P. 115578 - 115578

Published: Jan. 1, 2025

Language: Английский

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Efficient urea removal with hydroperoxide production in bipolar membrane electrochemical cell using MoNiOOH nanoarray anode electrocatalyst

Applied Catalysis B Environment and Energy, Journal Year: 2025, Volume and Issue: unknown, P. 125158 - 125158

Published: Feb. 1, 2025

Language: Английский

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Electrochemical Pilot H₂O₂ Production by Solid‐State Electrolyte Reactor: Insights From a Hybrid Catalyst for 2‐Electron Oxygen Reduction Reaction

Angewandte Chemie International Edition, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

The electrochemical oxygen reduction reaction (ORR) offers an alluring and sustainable alternative to the traditional anthraquinone process for hydrogen peroxide (H₂O₂) synthesis. However, challenges remain in developing scalable electrocatalysts cost-effective reactors high-purity H₂O₂ production. This study introduces a simple yet effective mechanical mixing method fabricate hybrid electrocatalyst from oxidized carbon nanotubes layered double hydroxides (LDHs). easily accessible low-cost catalyst achieves near-perfect Faradaic efficiency (∼100%) with low overpotentials of 73 mV at 10 mA cm⁻2 588 400 solid electrolyte cell. Through theoretical calculations in-situ analyses, we uncover pivotal role played by LDH co-catalyst fine-tuning local pH catalyst/solid-electrolyte interface that drives both activity selectivity. We also design solid-state reactor using cation-exchange resin (CER) as proton conductor microchannel efficient mass transfer, achieving production rate 5.29 mmol h⁻¹ continuous output concentrations 11.8 wt.% H₂O₂. Scaled industrial area 2 × 100 cm2, pilot impressive approximately 127.0 15 A, marking significant advancement

Language: Английский

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Dual‐Functional Catalyst of Amorphous TiO₂ Embedded in Mesoporous Carbon Hollow Spheres for H₂O₂ Electrosynthesis

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

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Electrochemical Pilot H₂O₂ Production by Solid‐State Electrolyte Reactor: Insights From a Hybrid Catalyst for 2‐Electron Oxygen Reduction Reaction

Angewandte Chemie, Journal Year: 2025, Volume and Issue: unknown

Published: March 10, 2025

Abstract The electrochemical oxygen reduction reaction (ORR) offers an alluring and sustainable alternative to the traditional anthraquinone process for hydrogen peroxide (H₂O₂) synthesis. However, challenges remain in developing scalable electrocatalysts cost‐effective reactors high‐purity H₂O₂ production. This study introduces a simple yet effective mechanical mixing method fabricate hybrid electrocatalyst from oxidized carbon nanotubes layered double hydroxides (LDHs). easily accessible low‐cost catalyst achieves near‐perfect Faradaic efficiency (∼100%) with low overpotentials of 73 mV at 10 mA cm⁻ 2 588 400 solid electrolyte cell. Through theoretical calculations in‐situ analyses, we uncover pivotal role played by LDH co‐catalyst fine‐tuning local pH catalyst/solid‐electrolyte interface that drives both activity selectivity. We also design solid‐state reactor using cation‐exchange resin (CER) as proton conductor microchannel efficient mass transfer, achieving production rate 5.29 mmol h⁻¹ continuous output concentrations 11.8 wt.% H₂O₂. Scaled industrial area × 100 cm , pilot impressive approximately 127.0 15 A, marking significant advancement

Language: Английский

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Highly Ordered Conductive Metal‐Organic Frameworks with Chemically Confined Polyoxometalate Clusters: A Dual‐Functional Electrocatalyst for Efficient H₂O₂ Synthesis and Biomass Valorization

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

Published: March 18, 2025

Abstract The design of bifunctional and high‐performance electrocatalysts that can be used as both cathodes anodes for the two‐electron oxygen reduction reaction (2e − ORR) biomass valorization is attracting increasing attention. Herein, a conserved ligand replacement strategy developed synthesis highly ordered conductive metal‐organic frameworks (Ni‐HITP, HITP = 2, 3, 6, 7, 10, 11‐hexaiminotriphenylene) with chemically confined phosphotungstic acid (PW 12 ) nanoclusters in nanopores. newly formed Ni−O−W bonds resultant Ni‐HITP/PW modulate electronic structures Ni W sites, which are favorable cathodic 2e ORR to H 2 O production anodic 5‐hydroxymethylfurfural oxidation (HMFOR) 5‐furandicarboxylic (FDCA), respectively. In combination deliberately retained pores, dual‐functional composites enable rate 9.51 mol g cat −1 h an FDCA yield 96.8% at current density 100 mA cm −2 /cell voltage 1.38 V integrated ORR/HMFOR system, significantly improved than traditional ORR/oxygen evolution system. This work has provided new insights into rational advanced electrocatalytic systems green valuable chemicals.

Language: Английский

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Highly Selective Electrooxidation of Glycerol to Tartronic Acid Over a Single‐Atom Rhodium Catalyst Supported on Indium Oxide

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

Published: March 27, 2025

The electrooxidation of biodiesel-derived glycerol offers an effective approach for the sustainable production valuable C3 compounds. However, highly selective synthesis a specific compound, such as tartronic acid (TA), by remains big challenge due to competitive dehydrogenation between CαH2(OH) and CβH(OH). Herein this study reports electrochemical oxidation reaction (GEOR) TA, which is catalyzed single-atom rhodium catalyst supported on indium oxide (Rh1-In2O3) in alkaline medium. At potential 1.40 V versus reversible hydrogen electrode, Rh1-In2O3-catalyzed GEOR achieves optimal TA selectivity 93.2% productivity 4.6 mmol cm-2 h-1, outperforming all previously reported electrocatalytic systems GEOR. Experimental results, complemented density functional theory calculation, reveal that Rh improves facilitating hydroxyl active oxygen species greatly decreasing energy barrier process, thus resulting high selectivity. Furthermore, integrated electrolyzer, combining with evolution reaction, current 100 mA at cell voltage 1.50 V. A techno-economic analysis demonstrates economic feasibility system.

Language: Английский

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