CHEMICAL ENGINEERING SCIENCE
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2026
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IF 5.1
Yisiqi Li,Jinlong Wu,Xueru Zhao,Hongrui Liu,Wen Qiao,Feng Li,Jing Li
The two-electron water oxidation reaction (2e − -WOR) offers a sustainable route for hydrogen peroxide production, yet its practical application remains constrained by the low Faradaic efficiency of catalysts. In this work, we demonstrate a dual-path H 2 O 2 production mechanism using a novel membrane-free electrolyzer, integrating oxygen reduction at a commercial carbon cloth (cathode) and WOR at zinc-vacancy-rich Zn x TiO 3 (anode). Furthermore, through in situ spectroscopic characterization, we reveal how the zinc vacancy concentration in the Zn x TiO 3 anode modulates the adsorption strength of *OOH intermediates, where Zn 0.66 TiO 3 exhibits optimal binding energy for *OOH intermediates while avoiding over-stabilization that would trigger the competing four-electron pathway, leading to a H 2 O 2 Faradaic efficiency of 69% at 3.2 V vs. RHE and delivers a H 2 O 2 partial current density up to 223 mA cm −2 at 3.3 V vs. RHE. Ultimately, by combining defect engineering with optimized electrolyzer design, the integrated system demonstrates synergistic enhancement through continuous cathodic ORR and WOR, reaching an exceptional overall efficiency of 152% at 240 mA cm −2 , demonstrating remarkable efficacy for the degradation of tetracycline contaminants, with a degradation rate reaching 80%. This study establishes defect engineering as a powerful strategy for designing selective H 2 O 2 electrocatalysts.
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高影响因子
Green Carbon
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2026
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IF 14.2
Shihao Li,Xiaoyang Yue,Fei Huang,Qian Zhang,Xiao Huang,Jingjing Zhao,Luwei Bao,Yanjun Jiang
Unspecific peroxygenases (UPOs) enable the selective hydroxylation of inert C–H bonds using H 2 O 2 under mild conditions. However, their practical application is fundamentally limited by oxidative deactivation at elevated H 2 O 2 concentrations. Herein, a highly synergistic photobiocatalytic system is constructed by covalently immobilizing UPOs onto a Rh-complex-coordinated covalent organic framework (COF) to facilitate the in-situ generation of H 2 O 2 and sequential enzymatic utilization. Specifically, a COF featuring a pyridinic imine structure (COF PyIm ) is designed to precisely anchor Rh(III) complexes. Compared with its bipyridine-structured analog (COF Bpy ), COF PyIm provides more coordination sites and a shorter electron-transfer distance. Consequently, the photocatalytic H 2 O 2 synthesis rate reached 22.17 mM·g -1 ·h -1 , representing a performance improvement of approximately 40%. This enhancement is attributed to the optimized pyridine–imine coordination microenvironment, which promotes charge separation and electron transfer. Subsequently, UPO from Agrocybe aegerita ( Aae UPO) is covalently immobilized onto COF PyIm to yield Aae UPO@Rh-COF PyIm , which achieves efficient spatiotemporal coupling between in situ H 2 O 2 generation and enzymatic hydroxylation of the C–H bond. This integrated photobiocatalyst can achieve 90% yield, >99% enantiomeric excess ( ee ), and a turnover number of 41,666 in the asymmetric hydroxylation of ethylbenzene. It also exhibits excellent reusability (retaining 70.4% of its initial activity after six cycles) and broad substrate scope.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2026
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IF 19.7
Juan Long,Gui Yang,Yang Wu,Lin Wang,Yawen Xiao,Shiping Zhang,Huachao Che,Juhong Zhan,Xiaoyong Wu,Bin Huang,Fengzhi Jiang,Shaowen Cao,Xuejun Pan
Ultrathin g-C 3 N 5 with Na-K sites, N-vacancies, and –C N was synthesized. • CN-Na-K yields 4739.89 μmol‧g −1 ‧h −1 H 2 O 2 under aeration-free conditions. • –C N and N-vacancies synergistically boost π-electron delocalization. • Na-K dual sites drive both ORR and WOR pathways for H 2 O 2 production. Photocatalytic solar-driven H 2 O 2 synthesis offers a sustainable energy route but is often limited by the need for supplemental oxygen. To overcome barriers, a distinctive ultra-thin g-C 3 N 5 nanosheet with cyano groups (–C N), N-vacancies, and Na-K dual active sites (CN-Na-K) was structured for H 2 O 2 production in natural-oxygen-conditions (aeration-free). The introduction of the –C N function as an electron pump to construct an internal electric field (IEF) promoted charge separation. Simultaneously, N-vacancies broke the structural localization to enhance π-electron delocalization, creating high-speed channels for carrier transport. Crucially, the Na-K dual sites acted as catalytic centers that enabled the water oxidation reaction (WOR) by driving the formation of key intermediates (*O 2 , *OOH, and *OH), where Na + acted as a powerful electron sink, and K + promoted excited-state electrons and stabilized holes. Therefore, the –C N, N-vacancies, and Na-K dual active sites synergistically promoted an enhanced H 2 O 2 production rate of CN-Na-K (1260.03 μmol‧g −1 ‧h −1 in LED lamp and 4739.89 μmol‧g −1 ‧h −1 in Xe lamp) under aeration-free conditions. Besides, characterizations and density functional theory (DFT) calculations confirmed the CN-Na-K system produced H 2 O 2 via a dual-channel pathway for the oxygen reduction (ORR) and WOR. This work provides a systemic design for electronic delocalization and dual active site engineering to achieve efficient aeration-free H 2 O 2 production. Download: Download high-res image (262KB) Download: Download full-size image
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Linghui Tang,Yue Wang,Yan Dong,Yasushi Hasebe
Hydrogen peroxide (H 2 O 2 ), a common reactive oxygen species, not only plays an important role in biological systems but is also widely used in industry. Its concentration varies across biological and environmental samples, and elevated levels can be highly hazardous and toxic. In aquaculture and lake water environments, H 2 O 2 may even reach the millimolar level. In this work, a highly conductive hydrogel (HG) was synthesized using a one-pot method from 2-acrylamido-2-methyl-1-propanesulfonic acid (AMPS), methacrylamide (MAM), and 2-hydroxyethyl methacrylate (HEMA) as raw materials. This conductive HG was coated on a glassy carbon electrode (GCE) surface. The resulting HG-GCE shows amplified cathodic current response toward H 2 O 2 in the presence of dissolved oxygen (DO) in electrolyte at neutral and acidic condition. Interestingly, the reduction current toward H 2 O 2 was markedly higher than in deoxygenated (N 2 -saturated) buffer, where the HG–GCE exhibited almost no response. This indicates that dissolved oxygen (molecular O 2 ) is essential for the H 2 O 2 sensing process of the HG–GCE, which we attribute to an O 2 -assisted electrochemical–chemical–electrochemical (ECE) mechanism. First, the HG may provide suitable microenvironment for the electrochemical reduction of the dissolved oxygen, producing O 2 ·− radical. Then, the produced O 2 ·− reacts with H 2 O 2 , which might /produce electrochemically active intermediates (HO 2 · radicals and HO 2 − ). These intermediates are further reduced at the GCE surface, generating measurable cathodic currents at −0.5 to −0.8 V vs. Ag/AgCl. Furthermore, in addition to the above ECE reaction process, we speculate two kinds of disproportionation (DISP) reactions within the HG-layer, which regenerate the O 2 and the H 2 O 2 , leading to the repeated ECE process (i.e., DO-assised amplified-H 2 O 2 response at the HG-GCE). Based on this ECE/DISP mechanism, the resulting HG/GCE-based H 2 O 2 sensor exhibits a good linear range for detecting H 2 O 2 from 1-35 mM, with low detection limit of 100 μM and sensitivity of 35.99 μA mM cm −2 , in air-saturated electrolyte buffer (at pH 3). The sensor demonstrated excellent stability, maintaining efficient detection for up to 45 days. This study also provides a new direction for the detection of H 2 O 2 using hydrogel materials.
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高影响因子
MATERIALS RESEARCH BULLETIN
·
2026
·
IF 5.8
Hui Liu,ZongXin Zhang,Hui Zhao,Zhongzheng Gao,Tao Wu,Xixi Zhu,Qingyun Liu
C@MoS 2 @Ag 2 S heterojunction nanozyme was constructed. • C@MoS 2 @Ag 2 S presented exceptional peroxidase-like activity. • p-nitrophenol was efficiently degraded by C@MoS 2 @Ag 2 S through activating H 2 O 2 and PDS. In this study, a carbon-coated MoS 2 @Ag 2 S (C@MoS 2 @Ag 2 S) heterojunction nanozyme with superior peroxidase-like activity is prepared via heterojunction pre-construction followed by carbonization. The kinetic parameters toward H 2 O 2 are determined to be K m = 1.02 mM and V max = 38.08 × 10 −8 M·s −1 , and toward 3,3′,5,5′-tetramethylbenzidine (TMB) are K m = 0.14 mM and V max = 60.35 × 10 −8 M·s −1 . Notably, its affinity for H 2 O 2 is substantially higher than that of natural horseradish peroxidase (HRP, K m = 3.7 mM), and the catalytic efficiency (V max ) is also superior. Enhanced performance stems from three-component synergy improving electron transport, charge separation, and ROS generation. Through synergistically activating persulfate (PDS) and H 2 O 2 , SO 4 • ⁻ , •OH, and 1 O 2 are generated, which collectively degrade PNP, achieving 90% removal in 40 min. This study offers theoretical guidance for the controllable synthesis of biomass-derived carbon/metal sulfide heterojunction nanozyme and the design of dual-oxidant synergistic activation systems for degradation of organic pollutants. Download: Download high-res image (151KB) Download: Download full-size image
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高影响因子
Materials Today Energy
·
2026
·
IF 8.1
Hui Lu,Shuai Zhang,Tao Sun,Wei Wang,Wei Sun,Li Yan,Xueying Cheng,Chunbo Liu
The photocatalytic two–electron oxygen reduction reaction (2e - ORR) for hydrogen peroxide (H 2 O 2 ) production offers a green and sustainable alternative to the energy–intensive anthraquinone process. Donor–π–acceptor (D–π–A) conjugated polymer photocatalysts are suitable for this reaction because their electronic structures and visible–light absorption can be readily tuned. However, inefficient charge separation and limited ORR selectivity remain major challenges. Here, we regulate the donor unit in a D–π–A polymer comprising an alkynyl triazine acceptor and an alkynyl π–bridge by replacing the fluorenone (DBF) donor with thienothiophene (DBTT). The stronger electron–donating character of DBTT promotes spatial separation of the highest occupied and lowest unoccupied molecular orbitals, facilitating charge separation and suppressing carrier recombination. Consequently, TEPT–DBTT achieves an H 2 O 2 production rate of 2273 μmol g -1 h -1 under visible light, approximately six times higher than that of TEPT–DBF. This study demonstrates that donor–unit engineering effectively modulates spatial charge separation and enhances photocatalytic H 2 O 2 production, providing a molecular design strategy for efficient triazine–based D–π–A polymer photocatalysts.
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高影响因子
ANALYTICA CHIMICA ACTA
·
2026
·
IF 6.1
Xin Zhuang,Jing Lin,Jialun Lin,Ranxi Mo,Xinyan Zheng,Yiqing Chen,Yuhua Hu,Ruiyun You,Yudong Lu
Functionalized Au@Ag NRs were immobilized in a triple-network hydrogel for wearable SERS sweat sensing. • Three reporter-functionalized hydrogel channels enabled ratiometric SERS detection of azelaic acid, H 2 O 2 , and pH. • The ATPPZn hydrogel showed good signal uniformity, reproducibility, 100-day storage stability, and skin-contact adaptability. • Sensitive detection of azelaic acid and H 2 O 2 was achieved with detection limits of 7.8 × 10 −13 M and 66.1 μM, respectively. • Real sweat analysis confirmed the feasibility of the platform for monitoring skin-inflammation-related molecular changes. Skin inflammation is commonly accompanied by oxidative stress and changes in the local acid–base microenvironment, whereas molecular indicators reflecting inflammation-associated metabolic changes remain less explored in wearable sensing. Azelaic acid, a dicarboxylic acid associated with inflammatory skin conditions, represents a potential small-molecule target, yet its non-invasive analysis in sweat remains challenging. Herein, a wearable-compatible ratiometric surface-enhanced Raman scattering (SERS) platform was constructed by embedding functionalized Au@Ag nanorods into a TEMPO-oxidized cellulose nanofibers (TOCNF)/poly(vinyl alcohol) (PVA)/poly(acrylamide-co-acrylic acid) [P(AM-co-AA)]-Zn 2+ triple-network hydrogel. The hydrogel architecture promoted nanoprobe dispersion and immobilization while maintaining flexibility and signal stability, yielding a spatial SERS relative standard deviation (RSD) of 5.19% and 77% signal retention after 100 days. Using Au@4-ATP@Ag nanorods (NRs) containing 4-ATP as a Raman-responsive reporter, azelaic acid was quantified through the ratiometric I 1194 /I 1073 response over 1 × 10 −12 –1 × 10 −7 M, with a detection limit of 7.8 × 10 −13 M, and its analytical feasibility in sweat was further evaluated by spike-recovery analysis. To provide complementary information on inflammation-related microenvironmental changes, the same hydrogel architecture was further adapted for H 2 O 2 and pH sensing using Au@4-MPBA@Ag and Au@4-MBA@Ag NRs, respectively. The H 2 O 2 channel exhibited a concentration-dependent response over 1-500 μM, while the pH response agreed well with pH-meter measurements, with deviations within 0.07 pH units. These results demonstrate the analytical feasibility of azelaic acid as an underexplored inflammation-related sweat target and highlight the potential of the triple-network SERS hydrogel for integrating molecular and microenvironmental information in skin-related sweat analysis. Download: Download high-res image (313KB) Download: Download full-size image
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高影响因子
ACS Nano
·
2025
·
IF 16
Senyuan Jia,Jingchen Na,Xinyi Liu,Jiaxin Li,Shucheng Sun,Hongmei Yu,Zhigang Shao
The versatile neutral hydrogen peroxide (H2O2), synthesized via electrocatalytic oxygen reduction reaction (ORR), holds significant promise for various applications. However, there have been limited reports on catalysts that operate at ampere-level current densities. The insufficient research on catalysts has hindered advancements in the 2e– ORR. Understanding how the coordination environment of single-atom catalysts influences 2e– ORR performance is crucial. In this study, we adjusted the adsorption energy of the reaction intermediates on nickel single-atom sites by utilizing oxygen functional groups present on carbon supports. Through a combination of comparative experiments and theoretical calculations, we demonstrated that Ni sites regulated by hydroxyl groups through direct interactions serve as excellent 2e– ORR sites. The resulting nickel single-atom catalyst (NiTPP@CNT-ox) exhibited an impressive H2O2 selectivity of up to 97.0% during rotating ring-disk electrode tests conducted in a 0.1 M K2SO4 solution at 0.4 V (vs RHE). In a two-electrode flow cell equipped with the NiTPP@CNT-ox-loaded gas diffusion electrode, a Faradaic efficiency exceeding 92.1% was achieved at current densities ranging from 0.2 to 1 A cm–2. Furthermore, the current density reached an unprecedented level of 1.6 A cm–2 while maintaining a Faradaic efficiency of 86.2%. Through cyclic operation, a H2O2 concentration of 10.0 wt % was attained. When scaling up the electrode area to 40 cm2, it is possible to obtain H2O2 at a concentration of 3.62 wt % directly without necessitating electrolyte recycling, thereby satisfying the concentration requirements for medical applications.
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PubMed
高影响因子
ENVIRONMENTAL TECHNOLOGY
·
2025
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IF 2
Lei Chen,Yun Wang,Haiyang Shao,Chengkai Mao,Minghong Wu,Gang Xu
The increasing presence of benzothiazole (BTH) in industrial wastewater poses significant environmental and health risks due to its persistence and toxicity. This study compares UV/persulfate (UV/K₂S₂O₈) and UV/H₂O₂ systems for benzothiazole (BTH) degradation, revealing that UV/K₂S₂O₈ achieves complete BTH removal (100%, 0.189 min−1) versus 85% (0.092 min−1) for UV/H₂O₂ under identical conditions. Radical scavenging experiments and LC-MS analysis demonstrate sulfate radicals outperform hydroxyl radicals in oxidizing BTH heterocyclic structure, reducing intermediates by 63% (quantified via peak area ratios). pH-dependent kinetics show UV/K₂S₂O₈ maintains efficacy (90–100% removal) across pH 3–9, while UV/H₂O₂ efficiency drops to 58% at pH > 7. Practical validation in river water confirms UV/K₂S₂O₈ robustness (98% BTH degradation), positioning it as a scalable, energy-efficient solution for refractory pollutant treatment. The results showed that the oxidant concentration and pH affected the degradation rate of BTH by changing the free radical concentration, and the UV/ K2S2O8 was demonstrated to be able to achieve efficient removal of pollutants in complex environmental matrices. Free radical scavenging experiments and liquid chromatography-mass spectrometry analysis confirm that sulfate radicals are more effective than hydroxyl radicals in oxidizing and degrading BTH, enabling rapid, efficient, and environmentally friendly degradation of pollutants. This is mainly due to the higher redox potential of sulfate radicals (2.8–3.1V) compared to hydroxyl radicals (2.01V), resulting in the generation of fewer intermediates. Compared to UV/H2O2, UV/K2S2O8 is a more effective, cleaner, and energy-saving method for pollutant removal in various complex environmental matrices.
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PubMed
高影响因子
Molecular Catalysis
·
2025
·
IF 4.9
Wenhua Fu,Nan Li,Qian Dong,Gang Zhao,Shirui Zhang,Yi Wu,Kai Zhao,Jiangquan Ma
Photocatalytic production of hydrogen peroxide (H 2 O 2 ) and carbon dioxide (CO 2 ) reduction has been the hotspots in the field of chemical industry for a long time. CdIn 2 S 4 is widely used due to its excellent thermal stability and significant absorption in the visible light region. However, the low efficiency of photogenerated charge separation hinders its practical application. In this work, Z-scheme heterojunction ReS 2 /CdIn 2 S 4 was successfully synthesized by hydrothermal method and applied for the first time in photocatalytic production of H 2 O 2 and CO 2 reduction. The experimental results show that compared with pure CdIn 2 S 4 or pure ReS 2 , the photocatalytic performance of ReS 2 /CdIn 2 S 4 is greatly improved. When the loading amount of ReS 2 is 12 wt. % of CdIn 2 S 4 , it exhibits the optimal photocatalytic H 2 O 2 productivity of 361.8 μmol h -1 g -1 and the optimal yields of CO and CH 4 of 89.84 and 5.03 μmol h -1 g -1 respectively in pure water. The Z-scheme heterojunction of ReS 2 /CdIn 2 S 4 was determined by XPS and the band structure. In addition, two possible reaction pathways involving O 2 - and 1 O 2 were analyzed for the H 2 O 2 production by RS/CIS and the pathway of carbon dioxide reduction reaction can be speculated through in-situ DRIFTS.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Renzhi Xiong,Yiting Sun,Jiahao Huang,Fangde Liu,Yanhe Xiao,Baochang Cheng,Shuijin Lei
Photocatalytic production of H 2 O 2 faces challenges such as low charge separation efficiency, narrow light absorption, and sluggish reaction kinetics. This study developed a WO 3− x @Zn 3 In 2 S 6− x S-scheme heterojunction and designed atomic-level W S interface chemical bonds through a defect-induced strategy to address these challenges. Oxygen/sulfur vacancies not only promote the formation of chemical bonds but also trigger a local surface plasmon resonance effect (LSPR) in WO 3− x , enabling full-spectrum light harvesting and photothermal heating. The S-scheme charge transfer retains the high-energy electrons in Zn 3 In 2 S 6− x and holes in WO 3− x to realize dual H 2 O 2 generation pathways. Coupled with LSPR-induced thermal activation, this multidimensional strategy achieved an unprecedented H 2 O 2 yield (3891.2 μmol g −1 h −1 ) under simulated sunlight, which is 9.2 times and 161.5 times higher than that of the non-thermally activated pristine Zn 3 In 2 S 6− x and WO 3− x , respectively. In situ X-ray photoelectron spectroscopy and a series of photoelectrochemical measurements confirmed the S-scheme charge dynamics, and electron spin resonance verified the thermally enhanced reactive oxygen species generation. This work establishes defect-mediated heterointerfacial engineering as a universal paradigm for solar-to-chemical energy conversion and provides feasible insights for designing photothermal-assisted photocatalytic systems.
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高影响因子
ACS ES&T Engineering
·
2025
·
IF 6.7
Zhu Liang,Jianjun Zhang,Yingfei Sun,Xinyu Nie,Chengzhi Zhu,Kaimin Shih,Bohua Wen,Xiao-yan Li,Lin Lin
In addressing the expensive transportation and disposal cost of the waste activated sludge (WAS), an in situ sludge reduction strategy was developed in this study based on H2O2/O3 lysis and a cryptic growth process. The critical roles of sludge solubilization and biodegradability of sludge lysate were analyzed comprehensively. Under a dosage of 0.36 g O3/g mixed liquor volatile suspended solids (MLVSS), H2O2 addition (H2O2/O3 molar ratio was 0.25) led to a significant improvement of sludge cell lysis performance in terms of the MLVSS reduction ratio (35.2% vs 26.3%). Compared with O3 alone, the sludge lysate treated with H2O2/O3 exhibited a higher biodegradability, as the value of BOD5/COD increased from 0.72 to 0.79, accompanied by mean specific rates of 6.71 and 7.42 h–1, respectively. Reintroduction of the H2O2/O3-treated sludge into the mainstream biological process facilitated further hydrolysis of oxidized sludge fragments, achieving an overall sludge reduction ratio of 29.1% without adversely affecting the effluent quality adversely. A pilot-scale experiment at 2.4 m3/d treatment capacity also demonstrated a similar sludge reduction performance of 28.1% in term of MLVSS. Economic analysis revealed that the net benefit of the in situ sludge reduction reached 132/t dry sludge (DS), highlighting the significant potential of the combined H2O2/O3 method for effective sludge reduction.
研究领域:
环境工程
·
废水处理
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高影响因子
危险品化学品经营许可证（带存储）