Inorganics
·
2026
·Vol. 14
·期 9
·237
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IF 3.4
Qi Guo,Pan Hou,Jingjie Cao,Hui Liu,Ge Tian
The selective photocatalytic reduction of O2to H2O2is an attractive route for sustainable H2O2synthesis, yet its efficiency is often limited by the sluggish charge separation and insufficient selectivity of the two-electron oxygen reduction reaction. Here, we develop a conductive 2D Cu3(HHTP)2metal–organic framework (MOF) in which Cu2+sites serve as dynamic redox centers to regulate interfacial electron transfer and O2activation. Upon photoexcitation, photogenerated electrons are preferentially transferred to Cu centers, inducing reversible reconstruction of the local Cu coordination environment. Benefiting from the extended π-conjugated framework and strong interlayer electronic coupling, the accumulated electrons can delocalize over the 2D sheets, facilitating charge separation and suppressing electron–hole recombination. Spectroscopic and theoretical investigations further reveal that the dynamically reconstructed Cu sites promote O2adsorption and activation through electron donation from Cu d orbitals to O2antibonding states, thereby stabilizing the O2−intermediate and favoring the two-electron reduction pathway toward H2O2. As a result, the Cu3(HHTP)2photocatalyst achieves an H2O2evolution rate of 3910 μmol g−1h−1under visible-light irradiation. These findings demonstrate that dynamically regulated Cu electronic structures provide an effective strategy for coupling charge-carrier management with selective O2activation, offering a rational approach to the design of conductive 2D photocatalysts for efficient H2O2photosynthesis.
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Journal of Environmental Chemical Engineering
·
2026
·Vol. 14
·期 5
·123518
·
IF 7.5
Meiyuan Wu,Zi Li,Tong Li,Kelei Huang,Xiangchao Meng,Zizhen Li
Despite its potential as a visible-light-responsive photocatalyst, the practical application of BiOBr is hindered by rapid charge recombination and an insufficient number of surface-active sites. While crystal plane engineering can guide the directional migration of photogenerated carriers to specific facets, enhancing separation, this approach alone yields limited performance gains. To further boost photocatalytic H 2 O 2 production, this study employed a combined strategy of crystal plane regulation and Au nanoparticle loading. Notably, this simple metal modification not only facilitates charge separation but also induces a clear swap of the dominant reaction pathways on specific BiOBr facets. Specifically, Au loading transforms the primary role of the {010} plane from water oxidation to oxygen reduction for H 2 O 2 generation, while on the {001} plane, it shifts from oxygen reduction to water oxidation. Such a reciprocal switching of facet-specific functions via metal decoration has rarely been explored in BiOBr or similar layered photocatalysts. Remarkably, the Au-loaded BiOBr{010} achieved a H 2 O 2 production rate of 2273 μmol·h −1 ·g −1 , which is 15.5 times higher than that of the pristine counterpart. This dramatic enhancement is primarily due to the formation of Au δ+ species, which act as new active sites and significantly improve oxygen adsorption on the catalyst surface.
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KOREAN JOURNAL OF CHEMICAL ENGINEERING
·
2026
·
IF 3.4
Jiang Pengfei,Hao Yifan,Jia Mingxi,Liu Cun
Hydrogen peroxide (H 2 O 2 ) is a key reactive oxygen species involved in physiological regulation and pathological processes, and its accurate quantification is essential for bioanalysis and disease-related studies. Herein, we report the synthesis of a series of Cu-Fe oxide nanozymes via a simple antisolvent crystallization strategy and systematically investigate their peroxidase-like catalytic activity toward colorimetric H 2 O 2 detection. By tuning the Cu/Fe molar ratio, the catalytic activity of the nanozymes can be effectively regulated, with Cu 2 FeO x exhibiting the highest peroxidase-like activity toward 3,3′,5,5′-tetramethylbenzidine (TMB) oxidation in the presence of H 2 O 2 under acidic conditions and enabling sensitive colorimetric detection of H 2 O 2 over a linear range of 10–200 µM with a detection limit of 0.572 µM. Furthermore, the proposed sensing platform demonstrates satisfactory selectivity and reproducibility, and is successfully applied to the determination of H 2 O 2 released into cell culture supernatants after chemical stimulation. This work highlights the potential of composition‑regulated Cu-Fe oxide nanozymes as robust artificial enzymes for colorimetric H 2 O 2 sensing and provides insights into their application in bioanalytical systems.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Deli Jiang,Tianle Ren,Sirui Liu,Zhanzhen Ma,Qunhua Zhong,Yingxue Cui,Jianjun Zhu,Di Li
A novel all-organic AQ/CvCN photocatalyst is designed for H₂O₂ photosynthesis. • The optimal 20% AQ/C V CN shows 18-fold H₂O₂ photosynthesis activity over pristine CN. • The synergy of AQ/C V CN promotes charge transfer and O₂ adsorption-activation. • AQ/CvCN maintains stable H₂O₂ production activity after long-term cycling tests. Carbon nitrides (CN) have been extensively studied in hydrogen peroxide (H 2 O 2 ) photosynthesis research field owing to their remarkable stability and tunable structural properties. Nevertheless, the weak photogenerated carrier separation ability, the insufficient adsorption and activation of O 2 , and the high reduction potential for H 2 O 2 generation on CN limit their applications in photocatalytic H 2 O 2 production. Herein, we successfully prepared all-organic CN-based photocatalysts (AQ/CvCN) via combining CN with carbon vacancies (Cv) and anthraquinone (AQ) to overcome the above limitations, thereby enhancing photocatalytic H 2 O 2 production. Significantly, experimental results and theoretical calculations demonstrate that the introduced Cv can break the symmetrical structure of CN and act as electron capture sites, which remarkably enhances the photogenerated carrier separation and the adsorption and activation of O 2 , while the loading of AQ can optimize the reduction potential of O 2 to H 2 O 2 and reduce the formation energy barrier of the critical intermediate *OOH, therefore collaboratively improving the activity of photocatalytic H 2 O 2 production. The designed 20% AQ/CvCN catalyst achieved a photocatalytic H 2 O 2 production rate of 10,053.46 μmol g −1 h −1 , which is 18.16 and 5.58 times higher than that of CN and CvCN, respectively. In addition, 20% AQ/CvCN maintains stable H₂O₂ evolution activity after long-term cycling tests. This study provides an efficient, economical, and environmentally friendly approach for designing CN-based photocatalysts used in photocatalytic H 2 O 2 production. Download: Download high-res image (367KB) Download: Download full-size image
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JOURNAL OF ELECTRONIC MATERIALS
·
2026
·
IF 2.8
Dai Han Yan,Xu Jing Wen,Zeng Han
In this work, we made a ternary composite made up of polydopamine-modified carbon nanotubes and Au nanoparticles that acts as a unit to hold a redox protein. The components within the ternary complex serve as a cofactor orientation guide, a conductive element, and an electron shuttle promoter, respectively. The electrochemical reactions occurring at this electrode were dominated by the redox process of the active cofactors in hemoglobin in coordination with polydopamine, achieving favorable efficiency with charge transfer of 69.8 s −1 . The hemoglobin-based electrode displayed an efficient electrocatalytic effect toward H 2 O 2 reduction with an onset potential of 0.058 V, close to the formal potential value for heme sites on hemoglobin. The normalized turnover frequency of the substrate in hemoglobin-induced electrocatalysis was estimated to be 7.0 × 10 2 s −1 . The as-prepared hemoglobin-based electrode exhibited favorable affinity, appropriate sensitivity, and a moderate detection limit toward the substrate ( K M = 0.214 mM, 1.01 × 10 −3 A·L·mol −1 , and 5.0 × 10 −3 mmol·L −1 ). The substrate diffusion process was identified as the key factor limiting the electrocatalytic performance of the hemoglobin-based electrode (2.23 × 10 −2 s −1 ). A glucose–H 2 O 2 biofuel cell was fabricated and could operate at an open-circuit potential of 0.72 V. Such a cell could produce a desirable power output density of ~5500 μW·cm −2 in the presence of a proton exchange membrane. Graphical Competitive ligation of heme protein with polydopamine could play a protective role against the negative effect of direct contact of the enzyme molecule with Au nanoparticles to retain the original configuration of native hemoglobin and exert its underlying electrocatalytic activity.
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Nature Communications
·
2026
·
IF 18.1
Wang Yifei,Duan Peiyang,Liao Yingqi,Wang Hao,Li Beibei,Zhang Hangyuan,Yang Hao,Cheng Tao,Sun Jingyu
Electrocatalytic oxygen reduction reaction (ORR) for H 2 O 2 production represents a sustainable alternative route to the energy-intensive anthraquinone process. Nevertheless, under industrially-relevant acidic conditions, excessive protons at the reaction interface exacerbate low H 2 O 2 selectivity and severe H 2 O 2 reduction. Herein, we propose a universal alkali metal cation (AMC: Li + , Na + , K + , or Cs + ) dosing strategy to markedly boost the acidic H 2 O 2 electrosynthesis. Upon Cs + addition, 2e − ORR selectivity increases from 20% to 80%, concurrently suppressing an H 2 O 2 reduction current by 50% and achieving an H 2 O 2 production rate of 9.2 mol g −1 h −1 at 500 mA cm −2 . Microelectrode hydrogen evolution measurements witness impeded proton diffusion in AMC-dosed acidic electrolytes, directly restricting proton supply to catalytic active sites. In situ spectroscopic analysis combined with molecular dynamics simulation demonstrate AMCs help reconfigure interfacial water networks via cation hydration shells, thereby disrupting proton-hopping pathways. The efficacy trend (Li +
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APPLIED SURFACE SCIENCE
·
2026
·
IF 6.6
Xuanyu Wang,Han Zhong,Xuanling Liu,Jianfei Yang,Ziling Zhang,Jiazheng Su,Jinxian Lee,Han Wang,Qiang Luo,Hong Lin
Modifying the surfaces of photocatalysts with organic cocatalysts is effective in promoting the photosynthesis of hydrogen peroxide (H 2 O 2 ), a versatile oxidant and environmentally benign fuel. Although the configuration of organic molecules dictates their properties and performance, it has not been discussed in organic-cocatalyst-modified photocatalysts. Herein, in order to study this potential influence on H 2 O 2 photosynthesis, we have managed to prepare tetracyanoquinodimethane (TCNQ)-modified silver thiogallate (AgGaS 2 ) nanoclusters with two different surface configurations via an active photodeposition strategy pioneered in this work (T/A-light) and a conventional stirring-adsorption process in the dark (T/A-dark). It has been confirmed that TCNQ adopts an end-on configuration and serves as a surface-coordinated molecular cocatalyst with a surface charge-transfer doping effect in T/A-light, whereas it takes a face-to-face geometry and establishes a heterojunction in T/A-dark. Moreover, T/A-light displays better light absorbance, oxygen adsorption and activation, H 2 O 2 selectivity, and photocatalytic activity with small amount of TCNQ (ω(TCNQ)); while its performance is overtaken by T/A-dark as ω(TCNQ) increases via multilayer adsorption which further strengthens interfacial electric fields and facilitates the charge separation and H 2 O 2 desorption. The highest production rate reaches 2.11 mmol g −1 h −1 , which is nearly four times that of pristine AgGaS 2 and better than that of most counterparts. This work has shed light on the configuration-dependent performance of organic cocatalysts and concurrently expanded the concept and application of photodeposition, offering a significant insight into designing high-performance surface-modified photocatalysts.
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ACS Sustainable Chemistry & Engineering
·
2026
·
IF 7.6
Jinbao Li,Jialin Zhang,Chi Zhang,Qiao Yao,Xuan Zhao,Li Ma,Jing Bai,Yunting Liu,Yanjun Jiang,Guanhua Liu
Abstract Unspecific peroxygenase (UPO) catalyzes selective oxyfunctionalization of C–H bonds using H2O2 but suffers from enzyme instability and substrate solubility issues. To address these challenges, a cobalt and nitrogen co-doped carbon nanotubes electrocatalyst with two-electron oxygen reduction performance was developed to electrocatalytically generate H2O2 in situ to avoid the damage from adscititious H2O2. This approach maintains the H2O2 concentration in the reaction system to balance the reactivity and oxidative inactivation of UPO. Meanwhile, a covalent organic framework (COF, TpTa) with good biocompatibility was selected as the carrier to prepare AaeUPO@TpTa immobilized enzymes, enhancing enzyme stability and substrate enrichment. By integrating the in situ H2O2 generation system via electrocatalysis with immobilized enzyme catalysis, and using 4-ethylbenzoic acid as a model substrate, the reaction achieved a 99.1% yield of 4-(1-hydroxyethyl)benzoic acid after 16 h, with broad substrate applicability and excellent enantioselectivity (94–99% ee). The constructed electroenzymatic cascade catalysis system enables efficient C–H bond hydroxylation.
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ACS Catalysis
·
2025
·
IF 13.1
Shuangshuang Wei,Wentao Zhang,Ziyi Wang,Guoyang Zhang,Wen-Wei Li,Guixiang Zeng,Shujuan Zhang
Nanozymes, while possessing greater stability and durability than their natural counterparts, still face limitations of low catalytic activity and inefficient production. Here, we report a one-step method for the efficient construction of highly active nanozymes. The photolysis of butanedione was leveraged to generate surface-functionalized metal nanozymes. The in situ generated surface acetate (Ac) ligands serve as electron bridges between the substrates to boost the electron transfer, thus drastically improving the catalytic activity. The resulting Ac-Ptzyme, with a precisely tuned surface Ac content, demonstrated a peroxidase-like activity superior to that of the natural horseradish peroxidase and was approximately 200 times greater than that of Fe3O4. This superior activity endowed the Ac-Ptzyme with enhanced performance for visually monitoring the oxidative stress in bloom-forming cyanobacterial cells and for killing pathogenic bacteria in biofilm. This work paves a path to the facile synthesis of high-activity nanozymes for catalysis.
研究领域:
生物化学
·
纳米医学
·
催化科学
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Simin Zhang,Jiawei Xu,Jiayong Lu,Zhijian Liu,Zechen Xiao,Wei Guo,Mo Zhang,Yan Wan,Yangming Lin
Covalent organic frameworks (COFs), as a class of emerging porous crystalline polymers with high specific surface areas and tunable framework structures, exhibit great potential in oxygen reduction reaction (ORR). Herein, we synthesize a series of benzothiophene-based COFs with varying benzene ring counts in the linkers and employ these materials to unveil the correlation between conjugated structure and the selectivity toward H2O2 electro-synthesis. Experimental results display that the highest H2O2 selectivity (~90%) is offered by the benzothiophene-based COF bearing one benzene ring in the linker, exhibiting a negative correlation with the number of benzene rings in the linker. Theoretical calculations reveal that variations in the number of benzene rings modulated the adsorption strengths and sites of key reaction intermediates, thereby altering 2e- ORR pathway. The decrease in benzene ring count enable the dominant pathway for 2e- ORR become the H2O2 formation through the nucleophilic attack of the active *O2- species, which originates from the electron transfer of 3O2, on the carbon atom near the sulfur atom of the thiophene ring. This work highlights the importance of appropriate linkers and provides valuable insights for devising metal-free COF electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化科学
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Chen Shu,Bin Chen,Weihu Zhang,Lele Cui,Wenheng Jing
Renewable electricity-driven hydrogen peroxide (H 2 O 2 ) electrosynthesis technology has recently emerged as a multidisciplinary research frontier as its distributed deployment capability can provide enhanced versatility for various potential niche applications. Despite significant progress in screening advanced electrocatalysts and fundamental understanding of microscopic reaction mechanisms, industrially viable electrolysis devices suitable for this technology are still lacking due to technical challenges such as low space/electrode utilisation and single-pass yield as well as poor operability. Here, we demonstrate a membrane-free dual-cathode stack reactor featuring compactness (inter-electrode distance configured to flow field plate thickness) and ideal electrode utilisation (two cathodes paired with one anode). Structurally discontinuous carbon films with self-sustained aeration are assembled as cathodes, which enables open air-fed O 2 -to-H 2 O 2 conversion and thus effectively simplifies operation. Even with low electrolyte concentrations (0.05 M Na 2 SO 4 ), this design demonstrates efficient H 2 O 2 production from bench- to industrial-scale operating current densities (75–200 mA cm −2 ) at relatively low cell voltages (5.9–11.0 V). Impressive single-pass H 2 O 2 accumulations of 959.6–2332.1 mg L −1 with current efficiencies of 55.1 %–90.7 % can be achieved at low hydraulic retention times of 15–60 s. The practicality and reliability of the device can be further elucidated by its robustness in decentralized wastewater remediation scenarios. This all-material/components-commercial design paves the way for advancing the technology readiness level of H 2 O 2 electrosynthesis processes.
研究领域:
化学工程
·
环境科学
·
材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Wenya Tang,Zhuwei Li,Xiaoran Shi,Dongxuan Zhang,Dingfeng Jin,Yuanqing Li,Huitao Fan,Bo Li,Liya Wang,Jungang Hou
Artificial photosynthesis is a promising way to change light energy into chemical energy stored in hydrogen peroxide (H 2 O 2 ). However, numerous heterojunction-based photocatalytic systems have substantially restricted effective H 2 O 2 generation due to the intrinsic tendency toward fast charge recombination and the deficiency in active site population on the catalyst surface, especially under conditions not employing sacrificial agents. This study in situ prepared ZnIn 2 S 4 (ZIS) nanoflowers onto a hollow covalent organic framework to strategically engineer a type-II organic–inorganic core–shell heterojunction photocatalyst, transforming O 2 into H 2 O 2 . The heterojunction photocatalyst exhibited an exceptional H 2 O 2 productivity of 3334μmol g −1 h −1 when no sacrificial agent was added, surpassing most reported systems. Mechanistic studies revealed that the heterojunctions extended the light absorption spectrum toward longer wavelengths and significantly increased the probability of electron transfer from photogenerated carriers to reactive species, which accelerated the reduction of O 2 to H 2 O 2 . Furthermore, theoretical calculations confirmed that the heterojunction formation modified the coordination environment of the active sites on ZIS, fine-tuned the binding interaction between O 2 and the catalyst interface, and reduced the energy barrier of intermediates, leading to superior performance. This study designed a novel, highly efficient organic–inorganic core–shell heterojunction photocatalyst and provided a promising strategy for enhancing the O 2 -to-H 2 O 2 conversion.
研究领域:
化学
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材料科学
·
环境科学
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