CHINESE JOURNAL OF CATALYSIS
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2026
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IF 17.2
Ran Sun,Yuqi Zhang,Kunge Hou,Yujie Tan,Xingang Liu,Jianyuan Hou,Weixuan Zhao,Andrew E.H. Wheatley,Renxi Zhang
The photocatalytic efficiency of covalent organic frameworks (COFs) toward sustainable H 2 O 2 synthesis via oxygen reduction reaction (ORR) is intrinsically constrained by compromised proton-coupled electron transfer (PCET) dynamics, where retarded water oxidation reaction kinetics and exogenous proton donor dependence create a dual kinetic-thermodynamic constraint. This work presents a precision hydrogen–bond engineering strategy through the radio-frequency plasma modification of COF linkages, establishing a hydrogen–bond strength gradient (OH···N vs. SH···N) to probe the structure-function interplay that modulates PCET pathways. Systematic investigations reveal that hydrogen–bond strengthening at imine linkages enables dual functionality: creating both dynamic proton reservoirs and more accessible proton conduction pathways. This synergistic regulation reduces the energy barrier for direct 2e − ORR by 19.6% while suppressing high-energy intermediates in stepwise pathways, as confirmed by experiments and density functional theory calculations. The optimized SH-COF with appropriately stronger hydrogen bonds achieves exceptional photocatalytic H 2 O 2 production: 2.97 and 4.70 times that of corresponding OH-COF and pristine COF, respectively. Integrated crystal orbital Hamilton population analysis quantitatively correlates hydrogen–bond strength with charge transfer efficiency, establishing a relationship between hydrogen–bond energy and PCET kinetics. Our findings not only demonstrate plasma modification as an effective strategy for post-synthetic hydrogen–bond tuning but fundamentally advance the understanding of how hydrogen-bond thermodynamics govern PCET mechanisms.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Jie Wang,Yue Wang,Tong Tian,Xiaolin Song,Daochuan Jiang,Yupeng Yuan
Achieving high crystallinity in polymeric semiconductors is crucial for enhancing charge transport and optoelectronic performance. However, this remains a challenge due to the inefficiency of energy coupling during polymerization. Here, we introduce a precursor-polarization approach to improve the crystallinity of polymeric carbon nitride. By protonating the melem precursor, we generate highly polar -NH 3 ⁺ edge groups that significantly increase the microwave response and facilitate directional thermal activation during polycondensation. This polarization-mediated energy coupling accelerates the condensation process, yielding carbon nitride with improved crystallinity and charge transport properties. As a result, the material exhibits a tenfold increase in photocatalytic H 2 O 2 production compared with conventional microwave-generated carbon nitride, with an apparent quantum efficiency of 5.63% at 420 nm. Importantly, the photogenerated H 2 O 2 is directly applied to dissolve spent LiCoO 2 cathodes, demonstrating a solar-driven, environmentally benign strategy for lithium-ion battery recycling. This study establishes precursor polarization as a general design principle for controlling the crystallization of polymeric semiconductors and translating their optoelectronic advantages into sustainable chemical process.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2026
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IF 12.2
Yiqun Cao,Huiying Xuan,Jun Liu,Hao Li,Peng Zhang,Tianzeng Chen,Yonghong Wang,Biwu Chu,Pengfei Liu,Yujing Mu,Qingxin Ma,Hong He
H2O2 is a vital atmospheric oxidant, while its photolysis in the troposphere is negligible in conventional view. For the first time, we find that gas-phase H2O2 can undergo heterogeneous photolysis to produce OH radicals on the surfaces of particles such as SiO2, Fe2O3, and Na2SO4 under solar irradiation, which further convert NO to produce HONO and NO2. It is demonstrated that acidity can inhibit the formation of HONO and promote the formation of NO2 significantly. Moreover, the heterogeneous photolysis of H2O2 is dependent on the reactivity of particles, with inert surfaces being more conducive to the generation of OH radicals. A MCM box model indicates that the HONO formation rate via the H2O2 heterogeneous reaction can reach 0.10 ppb·h–1 at 9 a.m., and the relative contribution to the total daytime HONO production can account for approximately 5% at 1 p.m. Given the ubiquitous presence of SiO2 in mineral dust particles, glass curtain walls, and terrestrial soils, these findings indicate that heterogeneous photolysis of H2O2 on the particle surface could be a potential source of daytime HONO. Our research also underscores the importance of atmospheric interfacial chemistry and its contribution to unknown sources of atmospheric oxidizing capacity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2026
·
IF 9.6
Shuangyuan Liu,Xinyu Li,Yubei Xiong,Ting Wang,Cong Pan,Chuanyin Liu,Ping He,Shilong Li
In the field of advanced oxidation processes, the efficient activation of hydrogen peroxide (H 2 O 2 ) plays a crucial role in the degradation of organic pollutants. Herein, sulfur-doped CuFeO 2 (S-CuFeO 2 ) was synthesized and exhibited enhanced catalytic activity for sulfamethoxazole (SMX) degradation via H 2 O 2 activation. Sulfur incorporation into the CuFeO 2 lattice modulates the electronic structure and surface properties, thereby facilitating H 2 O 2 activation and promoting O O bond cleavage and the generation of highly reactive oxygen species (ROSs). Combined quenching experiments, electron spin resonance (ESR), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) calculations reveal that hydroxyl radicals (HO • ) and superoxide radicals (O 2 •− ) dominate the SMX degradation in oxidation process. In addition, the S-CuFeO 2 /H 2 O 2 system demonstrates good stability, low metal leaching, and effective performance in different water matrices and for various organic pollutants. Toxicity evaluation further indicates a reduction in overall toxicity during degradation. This work provides mechanistic insight into H 2 O 2 activation by sulfur-doped catalysts and offers a feasible strategy for designing efficient catalysts for antibiotic-contaminated wastewater treatment. Download: Download high-res image (199KB) Download: Download full-size image
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
·
IF 19.7
Wenrui Dai,Shao Zhang,Shuangjun Li,Haoran Du,Jiajia Gao,Shuning Xiao,Pengfei Xia,Shan Hu,Hexing Li,Xiaoyan Liu,Ru Zheng,Dieqing Zhang
A metal-free PEI/Nv-C 3 N 4 photocatalyst enables efficient gas-phase NO oxidation via an in situ photo-self-Fenton process. • Nitrogen vacancies and PEI cooperatively regulate interfacial electronic structure, O 2 activation, and proton-coupled electron transfer. • PEI functionalization switches ROS evolution from a ·O 2 ⁻ pathway to an H 2 O 2 /·OH-dominated oxidation pathway. • PEI/Nv-C 3 N 4 achieves 85% NO removal, 98.4% nitrate selectivity, and stable operation over 800 min under visible light. Photo-Fenton processes are highly effective for pollutant degradation, yet their application to gas-phase NO oxidation remains limited by metal leaching, external H 2 O 2 addition, and inefficient oxidant utilization. Herein, we develop a metal-free photocatalyst based on polyethyleneimine-functionalized nitrogen-vacancy-rich graphitic carbon nitride (PEI/N v -C 3 N 4 ) for efficient NO oxidation via an in situ photo-self-Fenton process under visible light irradiation. Nitrogen vacancies serve as the primary sites for O 2 adsorption and activation, while PEI functionalization reconstructs the interfacial electronic structure by introducing defect-molecule coupled mid-gap states and a proton-rich microenvironment. This molecular-defect synergy alters the oxygen reduction pathway from a conventional one-electron route toward a selective two-electron process (O 2 → ⁎OOH → H 2 O 2 ), followed by efficient in situ H 2 O 2 activation into ·OH radicals. Simultaneously, PEI enhances NO adsorption and stabilizes NO-derived intermediates, facilitating their complete oxidation into nitrate. As a result, PEI/N v -C 3 N 4 achieves 85% NO removal efficiency, 98.4% nitrate selectivity, and stable operation over 800 min without introducing metal components. Combined experimental and theoretical analyses reveal a mechanistic transition from a ·O 2 - -dominated pathway to an H 2 O 2 /·OH-mediated photo-self-Fenton process. This work provides a general molecular-defect co-engineering strategy for regulating ROS evolution in metal-free photocatalytic systems toward sustainable air purification. Download: Download high-res image (170KB) Download: Download full-size image This research shows an in situ generation and activation pathway of H 2 O 2 enabled by metal-free catalysts, enhancing the efficient removal of gas phase NO via photo-self-Fenton reaction.
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BIOORGANIC CHEMISTRY
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2026
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IF 5.1
Han Liu,Ning-Xi Wu,Si-Jin Zuo,Ru Yan,Hao-Xiang Jiang
This work presents LH, a hemicyanine-based activatable fluorescent probe for the sensitive detection of hydrogen peroxide (H 2 O 2 ). LH undergoes H 2 O 2 -triggered cleavage of the boronate recognition unit, resulting in a turn-on near-infrared (NIR) fluorescence response. The probe exhibited favorable sensitivity, with a limit of detection (LOD) of 0.04 μM, as well as good selectivity and biocompatibility under the tested conditions. Cellular imaging experiments demonstrated that LH could monitor intracellular H 2 O 2 changes in ovarian-derived cells. Furthermore, LH was applied to PCOS-model mice and serum samples, where enhanced fluorescence signals were observed compared with healthy controls, suggesting increased H 2 O 2 -associated oxidative changes in the PCOS model. These results indicate that LH may serve as a useful molecular imaging tool for studying oxidative stress-related changes in PCOS-model mice.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2026
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IF 19.9
Haochen Meng,Zhiyuan Sang,Qiao Jiang,Jing Wang,Hao Rao,Lin Wang,De'an Yang,Lichang Yin,Yuqian Qiao,Feng Hou,Ji Liang
Electrochemical hydrogen peroxide (H 2 O 2 ) synthesis in neutral saltwater holds promise for medical sterilization and marine remediation, but is limited by the scarcity of catalysts combining high selectivity and industrial-current capability. Here, we report a polythiophene-modulated strategy to activate the edge-nickel sites in the conductive metal-organic framework (Ni-HHTP) for efficient H 2 O 2 electrosynthesis via two-electron oxygen reduction reaction (2e − ORR). The polythiophene with sufficient oxygen-containing species in situ coordinated with the edge Ni-sites in Ni-HHTP to form a penta-coordinated Ni-O 5 configuration, thus tailoring the electronic structure of nickel centers and optimizing the 2e − ORR activity and selectivity. Meanwhile, Ni-HHTP possesses a well-defined porous architecture, in which polythiophene is incorporated and significantly enhances its electronic conductivity, favoring rapid reaction kinetics. Thus, the resulting catalyst achieves over 90% H 2 O 2 selectivity in simulated seawater (3.6 wt.% NaCl), and operates stably at an industrial current density of 250 mA cm −2 . When integrated into a solar-driven system, there is still an average Faradaic efficiency of ∼100% for H 2 O 2 electrosynthesis, as well as a solar-to-H 2 O 2 conversion efficiency of 12.8%. This work demonstrates the precise activation of metal sites in conductive metal-organic frameworks via polymer modulation, offering a practical avenue for industrial-scale H 2 O 2 electrosynthesis under neutral conditions.
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Molecular Catalysis
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2026
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IF 4.3
Jiarui Li,Bolun Mei,Zhouxuan Zang,Yi Yu,Guoji Liu,Li Xu
A series of Cr-UiO-66 catalysts with ligand-vacancy defects was prepared for the oxidative dehydrogenation of biomass-derived 1,2-propanediol to hydroxyacetone. • A volcano-shaped trend between defect level and hydroxyacetone yield was established. • Moderate ligand vacancies balance H 2 O 2 conversion and the selective formation of hydroxyacetone. • •OH radicals were identified as key species for H 2 O 2 -driven ODH of 1,2-propanediol. The oxidative dehydrogenation (ODH) of biomass-derived 1,2-propanediol (1,2-PDO) to the high-value chemical hydroxyacetone (HA) is a meaningful route for upgrading renewable feedstocks into value-added multifunctional chemicals. In this study, Cr-UiO-66 catalysts with tunable content of ligand vacancies were synthesized for the conversion of 1,2-PDO to HA. Notably, a volcano-shaped relationship was observed between defect density and HA yield. The optimized 0.4Cr-UiO-66 catalyst achieved an HA yield approximately 3 times that of pristine UiO-66, reaching 12.9% at 45 °C after 2 h. Moreover, the catalyst sustained its ODH performance over five reaction runs. Regulating the content of ligand vacancies was shown to modulate the acidic properties of Cr-UiO-66 and H 2 O 2 activation to generate •OH radicals. A moderate level of ligand vacancies enabled a balance between H 2 O 2 activation and selective HA formation, resulting in improved performance. This study highlights ligand-vacancy engineering as an effective strategy for regulating H 2 O 2 activation over UiO-66-based catalysts. It provides meaningful insights for tailoring structural defects in UiO-66 for the ODH valorization of biomass derivatives. Download: Download high-res image (159KB) Download: Download full-size image
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ACS Applied Energy Materials
·
2026
·Vol. 9
·期 14
·9390-9399
·
IF 5.5
Zhan Wenqi,Zhai Xingwu,Hu Jiaping,Xu Han-Shu,Tang Kaibin
Lithium−carbon dioxide (Li−CO 2 ) batteries are promising energy storage systems due to their high theoretical energy density and capability for CO 2 utilization, yet their practical performance is limited by sluggish reaction kinetics. Here, we report an effective edge-site engineering strategy to enhance the catalytic activity of MoS 2 nanosheets via controlled H 2 O 2 etching. Density functional theory (DFT) calculations reveal that edge sites exhibit significantly stronger adsorption toward key intermediates (Li, CO 2 , and Li 2 CO 3 ) than the basal plane, identifying them as dominant active centers. Guided by this insight, a series of MoS 2 nanosheets with tunable edge-site densities were synthesized on carbon paper. Structural characterizations confirm that moderate etching effectively increases edge-site exposure while preserving structural integrity. Electrochemical measurements demonstrate that the optimized MoS 2 -45 s electrode delivers a low overpotential of 0.77 V, excellent rate capability, and stable cycling over 700 h with an energy efficiency exceeding 75%. In short, our work highlights the critical role of edge-site regulation in improving catalytic performance and provides a rational strategy for designing advanced cathode materials for Li−CO 2 batteries.
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MICROCHEMICAL JOURNAL
·
2024
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IF 4.9
Zhiyu Gong,Yueyue Zhong,Minghong Fan,Weiming Fang,Zhengfei Yang
Metal-organic frameworks (MOFs), with a particular focus on zeolite-imidazole frameworks (ZIFs), have garnered significant interest as potential templates for the fabrication of sensing materials. In this work, we fabricated a porous stick structure of S-Co 3 O 4 /Co/C through the two-step pyrolysis of stick-like ZIF-67 (ZIF-S). Various methodologies were utilized to investigate the structures and composition of the nanocomposites. The S-Co 3 O 4 /Co/C was further utilized as electrode components in electrocatalytic determination of H 2 O 2 . Thanks to the unique stick-like structure and the synergistic effects of Co 3 O 4 , Co, and carbon, the fabricated sensor showed wide linear range (0.5–4000; 4000–11,000 μM), high sensitivity (1.01; 0.90 μA μM −1 cm −2 ) and low detection limit (0.29 μM) for H 2 O 2 sensing. The study being presented is anticipated to offer a novel outlook on the possible utility of nanocomposites derived from MOFs in the realm of electrochemical sensing.
研究领域:
材料科学
·
分析化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Da-Wei Wang,Ming-Yue Tian,Fang-Qi Wang,Xi-Wen He,Wen-You Li,Yu-Kui Zhang
Chemodynamic therapy (CDT) is an emerging treatment strategy that kills tumor cells by generating hydroxyl radicals (·OH) via the activation of Fenton/Fenton-like reactions within the tumor microenvironment (TME). Although CDT overcomes drug resistance issues and has minimal side effects, it still faces multiple challenges including low endogenous hydrogen peroxide (H 2 O 2 ) levels, inadequate catalytic efficiency, and targeting issues. To overcome these limitations, a novel precision-targeted responsive molecularly imprinted nanozyme (GZMIP) was developed. Using zeolitic imidazolate framework-8 (ZIF-8)-coated glucose oxidase (GOx) as a carrier (GZ) and the epitope of lactate transporter (MCT4) as the template, an imprinted layer was prepared on the GZ surface via radical polymerization reactions, followed by elution to obtain GZMIP. GZMIP targeted tumor cells with overexpressed MCT4. Upon entering cells, GZMIP occurred responsive cleavage in the acidic environment and GSH overexpressed TME, releasing GOx and copper(II) acrylate (CuA) monomers from the imprinted layer. GOx catalyzed intracellular glucose (Glu) to generate H 2 O 2 , while GSH reduced CuA to Cu + . The subsequent cascade reaction between Cu + and H 2 O 2 generated highly toxic ·OH, inducing cell death. Both in vitro and in vivo experiments demonstrated that GZMIP effectively inhibited tumor cell proliferation, showed a 75 ± 5 % growth inhibition rate in tumor-bearing mouse models, and exhibited excellent biocompatibility. This study innovatively integrated molecular imprinted polymers with nanozyme technology to establish a Fenton-like cascade catalytic system, simultaneously achieving precise delivery and controlled release of catalytic components. This approach significantly improving tumor targeting and therapeutic efficacy, providing a promising strategy for enhanced CDT.
研究领域:
纳米医学
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癌症治疗
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生物无机化学
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药物递送
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活性氧生物学
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高影响因子
JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Fengyi Wang,Hong Li,Shenshen Zhang,Bin Duan,Niu Huang,Yong Zheng,Binbin Jia,Siran Xu,Wei Liu,Liqun Ye
The development of non-noble metal catalysts with high activity and selectivity is critical for the electrocatalytic production of hydrogen peroxide (H 2 O 2 ). Herein, we report a composite catalyst (CTF/BHN) fabricated by chelating a basic bismuth salt (BHN) with a bipyridine-containing covalent triazine framework (CTF), forming strong Bi-bipyridine bonds at the interface. This catalyst exhibits exceptional H 2 O 2 selectivity (92–98 %) over a wide potential range (0.3–0.62 V vs. RHE). In H-type cell tests, it achieves a Faraday efficiency of 88.9 % at 20 mA cm −2 , with a high H 2 O 2 production rate of 1.65 mol g −1 h −1 , and maintains stable performance for 42 h. In-situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) and X-ray photoelectron spectroscopy (XPS) reveal that the superior performance stems from synergistic interfacial effects: electron transfer from BHN to CTF enhances charge transport, while polarized interfaces promote water dissociation and protonation of pyridine groups in CTF to form Py*H intermediates. Py*H acts as a proton relay, facilitating the protonation of adsorbed *O 2 to *OOH at Bi active sites. Concurrently, the enhanced interaction between *OOH and the catalyst surface (evidenced by the blue-shifted *OOH peak) stabilizes *OOH and suppresses its dissociation, thereby driving the 2e − ORR pathway for efficient H 2 O 2 generation.
研究领域:
电催化
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能源化学
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材料化学
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环境化学
·
分子催化
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