Construction of One-Dimensional Covalent–Organic Framework Coordinated with Main Group Metals for Selective Electrochemical Synthesis of H2O2 DOI
Jinyan Wang,

Huimin Sun,

Shaoda Huang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(42), P. 56459 - 56468

Published: Oct. 8, 2024

Covalent–organic frameworks (COFs) are promising electrocatalysts for the selective synthesis of H2O2 through two-electron oxygen reduction reaction (2e– ORR). However, design and efficient stable COF-based is still challenging. In this work, a predesigned 1,10-phenanthroline-based one-dimensional COF (PYTA-PTDE-COF) was constructed to anchor main group metal (In, Sn, Sb) as toward 2e– ORR. The catalysts featured with fully exposed metalated side chains. Structural characterization revealed that PYTA-PTDE-M's (M = In, all quite similar, except coordinated ions maintenance good crystallinity. They exhibited satisfying activity selectivity ORR under alkaline conditions. Among them, PYTA-PTDE-Sb best performance (Eonset 0.765 V, 96%, yield rate 209.2 mmol gcat–1 h–1). Moreover, it also delivered superior stability almost no attenuation current density during long-time test. Theoretical calculations Sb site in COFs has lowest adsorption strength *OOH, which could be reason its selectivity. assembled zinc–air battery realizes not only supply clean energy but production green chemicals, showing highly practical applications. This work offers an example designing metal-coordinated 1D reveals fundamental structure–activity relationship

Language: Английский

Recent strategies to improve the electroactivity of metal–organic frameworks for advanced electrocatalysis DOI Creative Commons

Runzhi Wei,

Xiao Li, Aziz B. Ibragimov

et al.

Deleted Journal, Journal Year: 2024, Volume and Issue: 1(2), P. 181 - 206

Published: Aug. 4, 2024

Abstract Metal–organic frameworks (MOFs) have emerged as promising materials in the realm of electrocatalysis due to their high surface area, tunable porosity, and versatile chemical functionality. However, practical application has been hampered by inherent limitations such low electrical conductivity a limited number active metal sites. Researchers addressed these challenges through various strategies, including enhancing incorporating conductive nanoparticles, modifying structure composition MOFs replacing nodes functionalizing linkers, preparing catalysts thermal processes decarburization conversion into oxides, phosphides (MPs), sulfides (MSs). This review provided comprehensive summary strategies that were employed enhance electroactivity for improved electrocatalytic performance recent years. It also explored future directions potential innovations design synthesis MOF‐based electrocatalysts, offering valuable insights advancing sustainable energy technologies.

Language: Английский

Citations

10

Functionalized Modification of Conjugated Porous Polymers for Full Reaction Photosynthesis of H2O2 DOI Open Access

Xiaobo Luo,

Shiyuan Zhou, Zhou Sheng

et al.

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 16, 2024

Abstract Modulating the molecular structure to achieve full reaction including oxygen reduction and water oxidation is a promising strategy for efficient photosynthesis of hydrogen peroxide (H 2 O ) but remains challenge. Herein, triphenylamine naphthalimide‐based conjugated porous polymers are synthesized with photo oxidation‐reduction structures, then sulfonate (─SO 3 H) quaternary ammonium groups introduced via post‐modification produce two photocatalysts named NI‐TPA‐NI‐SO H NI‐TPA‐NI‐N, respectively. Introducing charged functional has improved hydrophilicity (O adsorption, beyond that, ─SO further stabilizes adsorbed bonding as well accelerates photogenerated carrier separation electron/proton transport that enables . Therefore, motivated by charge separation, stabilized boosted proton‐coupled electron transfer, exhibits highest light‐driven production rate among three photocatalysts, reaching 3.40 mmol g −1 h , which 4.9‐fold NI‐TPA‐NI. Remarkably, in presence ethylenediaminetetraacetic acid disodium salt, its significantly enhances 14.5 superior most reported organic best knowledge.

Language: Английский

Citations

6

Highly efficient and mild synthesis of multimetallic metal–organic framework nanoparticles for enhanced oxygen evolution reactions DOI

Xinran Shi,

Sai‐Nan Guo,

Meng Qiao

et al.

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

Published: March 3, 2025

Abstract Multimetallic metal–organic framework (MOF) nanoparticles have been regarded as promising electrocatalysts for the oxygen evolution reaction (OER) due to their small size, porous structure, and synergistic active metal site. However, limitations such stringent preparation conditions, long times, low yields restrict further application. Herein, an instantaneous continuous approach is proposed synthesize multimetallic MOF utilizing high gravity technology. With greatly enhanced mixing mass transfer in rotating packed bed reactor, instantaneously synthesized bimetallic/trimetallic show smaller particle sizes, higher surface areas, OER performance compared with corresponding stirred tank reactor products. Density functional theory calculations elucidate intrinsic activity regulation mechanism of bimetallic MOFs. This study not only proposes efficient strategy MOFs but also can achieve scaled‐up ultra‐high space–time yield (43,700 kg m −3 day −1 ), promoting practical application electrocatalysis.

Language: Английский

Citations

0

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

Tong Bao,

You Wu, Chencheng Tang

et al.

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

Citations

0

Regulating the Local Reaction Microenvironment at Chromium Metal–Organic Frameworks for Efficient H2O2 Electrosynthesis in Neutral Electrolytes DOI Open Access
Zhihao Pei,

Yan Guo,

Deyan Luan

et al.

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

Published: March 30, 2025

Abstract The electrochemical synthesis of hydrogen peroxide represents a promising alternative to the traditional anthraquinone process, aiming for zero pollution. However, achieving efficient in neutral electrolytes is challenging due sluggish kinetics two‐electron oxygen reduction reaction. To address this issue, unique metal–organic framework (MOF) featuring Cr metal sites coordinated with tetrabromoterephthalic acid (Cr‐TBA) synthesized. This specially designed MOF exhibits distinctive paper‐clip‐like structure and remarkably enhanced Lewis acidity. Experimental results demonstrate that obtained can facilitate attraction OH − ions solution, promoting their accumulation on catalyst surface. enhancement leads excellent performances Cr‐TBA electrolytes, Faradaic efficiencies 96–98% production rate 13.4 mol g cat −1 h at current density 150 mA cm −2 . Operando spectroscopy functional theory calculations indicate modified microenvironment effectively facilitates conversion * OOH intermediates H 2 O

Language: Английский

Citations

0

Recent advances in green H2O2 production via metal-based functional materials: applications, strategies, and catalytic mechanisms DOI

Danhua Jiao,

Yongjun Li, Xiaodong Cai

et al.

Rare Metals, Journal Year: 2025, Volume and Issue: unknown

Published: April 15, 2025

Language: Английский

Citations

0

Engineering of Single‐Atomic Sites for Electro‐ and Photo‐Catalytic H2O2 Production DOI
Yunxiang Li, Deyan Luan, Xiong Wen Lou

et al.

Advanced Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Oct. 25, 2024

Direct electro- and photo-synthesis of H

Language: Английский

Citations

3

Electrocatalysts for the Formation of Hydrogen Peroxide by Oxygen Reduction Reaction DOI
Ke Yuan, Hong Li, Xiangyu Gu

et al.

ChemSusChem, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 6, 2024

Abstract Hydrogen peroxide (H 2 O ) is a widely used strong oxidant, and its traditional preparation methods, anthraquinone method, direct synthesis have many drawbacks. The method of producing H by two‐electron oxygen reduction reaction (2e − ORR) considered an alternative strategy for the due to high efficiency, energy saving, environmental friendliness, but it remains big challenge. In this review, we described mechanism ORR principle electrocatalytic performance testing, summarized standard evaluation techniques electrocatalysts produce . Secondly, according theoretical calculation experimental results, several kinds efficient are introduced. It concluded that noble metal‐based materials, carbon‐based non‐noble metal composites, single‐atom catalysts preferred catalyst materials 2e ORR. Finally, advantages novelty compared with methods production, as well disadvantages above‐mentioned high‐efficiency catalysts, summarized. application prospect development direction production has been prospected, which great significance promoting electrochemical yield developing green chemical production.

Language: Английский

Citations

2

Janus structural TaO/TaN heterojunction as efficient oxygen reduction electrocatalyst for H2O2 production DOI
Mei Li,

Ting Yang,

Wenling Du

et al.

Chemical Communications, Journal Year: 2024, Volume and Issue: 60(99), P. 14786 - 14789

Published: Jan. 1, 2024

A novel electrocatalyst composed of a Janus structured TaO/TaN heterojunction with graphene exhibits superior 2e − ORR activity, selectivity and durability in alkaline electrolytes, surpassing the comparative TaON@Gr.

Language: Английский

Citations

2

Construction of One-Dimensional Covalent–Organic Framework Coordinated with Main Group Metals for Selective Electrochemical Synthesis of H2O2 DOI
Jinyan Wang,

Huimin Sun,

Shaoda Huang

et al.

ACS Applied Materials & Interfaces, Journal Year: 2024, Volume and Issue: 16(42), P. 56459 - 56468

Published: Oct. 8, 2024

Covalent–organic frameworks (COFs) are promising electrocatalysts for the selective synthesis of H2O2 through two-electron oxygen reduction reaction (2e– ORR). However, design and efficient stable COF-based is still challenging. In this work, a predesigned 1,10-phenanthroline-based one-dimensional COF (PYTA-PTDE-COF) was constructed to anchor main group metal (In, Sn, Sb) as toward 2e– ORR. The catalysts featured with fully exposed metalated side chains. Structural characterization revealed that PYTA-PTDE-M's (M = In, all quite similar, except coordinated ions maintenance good crystallinity. They exhibited satisfying activity selectivity ORR under alkaline conditions. Among them, PYTA-PTDE-Sb best performance (Eonset 0.765 V, 96%, yield rate 209.2 mmol gcat–1 h–1). Moreover, it also delivered superior stability almost no attenuation current density during long-time test. Theoretical calculations Sb site in COFs has lowest adsorption strength *OOH, which could be reason its selectivity. assembled zinc–air battery realizes not only supply clean energy but production green chemicals, showing highly practical applications. This work offers an example designing metal-coordinated 1D reveals fundamental structure–activity relationship

Language: Английский

Citations

0