Tailoring Oxygen Reduction Reaction Pathway on Spinel Oxides via Surficial Geometrical‐Site Occupation Modification Driven by the Oxygen Evolution Reaction

Advanced Materials, Год журнала: 2022, Номер 34(28)

Опубликована: Май 13, 2022

The oxygen reduction reaction (ORR) has been demonstrated as a critical technology for both energy conversion technologies and hydrogen peroxide intermediate production. Herein, an in situ evolution (OER) surface strategy is applied changing the structure of MnCo2 O4 oxide with tetrahedral octahedral cations vacancies to realize pathway switching from 2e- ORR 4e- ORR. Interestingly, as-synthesized -pristine (MnCo2 -P) highest surficial Mn/Co octahedron occupation favors two electrons routes exhibiting high H2 O2 selectivity (≈80% reaches nearly 100% at 0.75 V vs RHE); after atoms reconstruction, -activation -A) largest tetrahedron present excellent performance through four-electron ultrahigh onset potential half-wave 0.78 0.92 V, ideal mass activity (MA), turnover frequencies (TOF) values. Density functional theory (DFT) calculations reveal concurrent modulations Co Mn by reconstructions, which improve electroactivity -A toward pathway. This work provides new perspective building correlation OER activation-ORR property, bringing detailed understating route transformation, thus guiding development certain electrocatalysts specific purposes.

Язык: Английский

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Strategies for Sustainable Production of Hydrogen Peroxide via Oxygen Reduction Reaction: From Catalyst Design to Device Setup

Nano-Micro Letters, Год журнала: 2023, Номер 15(1)

Опубликована: Май 9, 2023

Abstract An environmentally benign, sustainable, and cost-effective supply of H 2 O as a rapidly expanding consumption raw material is highly desired for chemical industries, medical treatment, household disinfection. The electrocatalytic production route via electrochemical oxygen reduction reaction (ORR) offers sustainable avenue the on-site from O. most crucial innovative part such technology lies in availability suitable electrocatalysts that promote two-electron (2e – ) ORR. In recent years, tremendous progress has been achieved designing efficient, robust, catalyst materials, including noble metals their alloys, metal-free carbon-based single-atom catalysts, molecular catalysts. Meanwhile, cell designs have significantly advanced applications at industrial level. This review summarizes fundamental basics advances 2e -ORR, design, mechanistic explorations, theoretical computations, experimental evaluations, designs. Perspectives on addressing remaining challenges are also presented with an emphasis large-scale synthesis route.

Язык: Английский

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Strategies and challenges on selective electrochemical hydrogen peroxide production: Catalyst and reaction medium design

Chem Catalysis, Год журнала: 2022, Номер 2(8), С. 1919 - 1960

Опубликована: Июнь 22, 2022

Язык: Английский

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Super‐Coordinated Nickel N₄Ni₁O₂Site Single‐Atom Catalyst for Selective H₂O₂Electrosynthesis at High Current Densities

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(38)

Опубликована: Авг. 2, 2022

Electrochemical production of hydrogen peroxide (H2 O2 ) from on single-atom catalysts has attracted great attention, yet the quest for robust is driven by achieving >90 % Faradaic efficiency (FE) under industrial-relevant current densities (>100 mA cm-2 ). Herein we synthesize a catalyst that contains single nickel site coordinated four nitrogen and two oxygen atoms (i.e., N4 Ni1 via involving carboxyl functionalized multiwall carbon nanotubes as substrate to provide extra O coordination regular NiN4 site. It cathodic energy approximately 82 H2 FE around 96 at 200 density, outperforming reported electrosynthesis.

Язык: Английский

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Extended Conjugation Tuning Carbon Nitride for Non‐sacrificial H₂O₂Photosynthesis and Hypoxic Tumor Therapy**

Angewandte Chemie International Edition, Год журнала: 2022, Номер 61(43)

Опубликована: Авг. 8, 2022

Abstract Artificial photocatalysis offers a clean approach for producing H 2 O . However, the poor selectivity and activity of production hamper traditional industrial applications emerging photodynamic therapy (PDT)/chemodynamic (CDT). Herein, we report C 5 N photocatalyst with conjugated C=N linkage selective efficient non‐sacrificial in both normoxic hypoxic systems. The strengthened delocalization π‐electrons by linkers downshifted band position, thermodynamically eliminating side evolution reaction kinetically promoting water oxidation. As result, had competitive solar‐to‐chemical conversion efficiency 0.55 % overall exhibited far highest under conditions (698 μM h −1 ). was further applied to PDT/CDT outstanding performance apparent cancer cell death synchronous bioimaging. study sheds light on photosynthesis carbon nitrides health applications.

Язык: Английский

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