ACS Catalysis
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2024
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IF 11.3
Xiaolong Tang,Changlin Yu,Jiaming Zhang,Kaiwei Liu,Debin Zeng,Fang Li,Feng Li,Guijun Ma,Yanbin Jiang,Yongfa Zhu
The limitations imposed by the high carrier recombination rate in the current photocatalytic H2O2 production system substantially restrict the rate of H2O2 generation. Herein, we successfully prepared an In2S3/HTCC dense heterojunction bridged by In–S–C bonds through in situ polymerization of glucose on In2S3. This interfacial In–S–C bond provides a fast transfer channel for electrons at the interface to achieve a highly efficient interfacial charge transfer efficiency, leading to the formation of an enhanced built-in electric field between In2S3 and HTCC, thus dramatically accelerating the rate of charge separation and effectively prolonging the lifetime of the photogenerated carriers. Moreover, the coverage of HTCC enhances the absorption of visible light and sorption of O2 by In2S3, while lowering its two-electron oxygen reduction reaction (ORR) energy barrier. Notably, our research demonstrates that In2S3/HTCC can generate H2O2 not only through the well-known two-step one-electron ORR but also via an alternative pathway utilizing 1O2 as an intermediate, thereby enhancing H2O2 production. Benefiting from these advantages, In2S3/HTCC-2 can produce H2O2 at a rate of up to 1392 μmol g–1 h–1 in a pure aqueous system, which is 18.2 and 5.2 times higher than that of pure In2S3 and HTCC, respectively. Our work not only provides a novel synthesis method of new organic/inorganic heterojunction photocatalysts based on HTCC but also offers new insights into the potential mechanism of interfacial bonding of heterostructures to regulate the photocatalytic H2O2 production activity.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2025
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IF 6.9
Xiaoying Xu,Shaofeng Dong,Jialong Lv,Guocheng Huang,Qiaoshan Chen,Jinhong Bi
The carrier transfer mechanism of S-scheme heterojunctions has been extensively explored, yet their impact on light absorption performance remains ambiguous. In this work, a finely designed S-scheme heterojunction was developed by coupling oxidation photocatalyst a specific covalent organic framework (COF)-TaTp, and reduction photocatalyst SnS 2 (SS) for in-situ H 2 O 2 photo-production and sterilization. The optimized 10% SS/TaTp achieved a 3.45- and 16.87-fold enhancement in H 2 O 2 generation than pure TaTp and SS, respectively, with significant improvements under visible and near-infrared (NIR) light. In-situ XPS, EPR, and Kelvin probe force microscopy (KPFM) verified the S-scheme charge transfer mechanism, underscoring accelerated photo-induced electrons migration and strengthened redox capacity. The internal electric field of 10% SS/TaTp was calculated to be 2.14 and 4.63 times stronger than TaTp and SS. Intriguingly, the electron localization function and partial density of states analyses revealed that the interfacial C-N-S covalent bonds finely tuned the energy band structure and generated hybrid energy levels in the heterojunction, thus improving light harvesting and catalytic performance in both visible-light and NIR region. This work highlights the role of interfacial covalent interactions in tuning energy levels in COF-based S-scheme photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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高影响因子
CHEMOSPHERE
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2024
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IF 8.1
Yizhuo Yang,Zhang Yan,Xin Luo,Jianxin Cao,Wenxiao Zheng,Chunhua Feng
The electrochemical treatment of saline wastewater is prone to the formation of inorganic chlorinated byproducts, being a significant challenge for this technology. In this study, we introduce an electrooxidation system utilizing a self-supporting nitrogen-doped carbon-based cathode embedded in carbon cloth (N@C-CC), designed to generate H₂O₂. This system aims to rapidly neutralize free chlorine produced at the anode, a precursor to inorganic chlorinated byproducts, thereby reducing their formation. Our results demonstrate that using the N@C-CC cathode in saline wastewater treatment yielded considerably lower concentrations of ClO₃⁻ and ClO₄⁻ (0.08 mM and 0.024 mM, respectively), which were only 20.5% and 22.7% of the levels produced using a Pt cathode without H₂O₂ generation. Moreover, the presence of cathodically generated H₂O₂ that quenches free chlorine did not significantly impact the degradation performance of phenol. Electron paramagnetic resonance tests and quenching experiments indicated that 1 O₂ was primarily responsible for phenol removal. Validation with real wastewater demonstrated reductions of 68.6% and 56.3% in ClO 3 − and ClO 4 − concentrations, respectively, while effectively removing other pollutants. This study thus offers a compelling method for mitigating the formation of inorganic chlorinated byproducts during the electrooxidation of saline wastewater.
研究领域:
环境科学
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化学工程
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PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2024
·Vol. 31
·期 27
·39439-39453
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IF 0
Liu Shitong,Wang Jun,Liu Yang,Yang Baojun,Hong Maoxin,Yu Shichao,Qiu Guanzhou
Red mud (RM) is a typical bulk solid waste with Fe/Al/Si/Ca-rich characteristics that has been used to prepare various heterogeneous catalysts such as iron-based catalysts and supported catalysts. Prussian blue analogues (PBA) is a low-cost, environmentally friendly, and active site rich iron-based metal organic framework, but its catalytic properties are adversely affected by their easy aggregation. In this study, nickel-doped RM-based PBA (RM-Ni PBA) was synthesized by acid dissolution-coprecipitation method for the degradation of ciprofloxacin (CIP). The characterization showed that RM-Ni PBA was a material with excellent dispersibility, large specific surface area, and abundant active sites. The degradation results showed that the removal efficiency of CIP in the RM-Ni PBA/H 2 O 2 system was 16.63, 1.78, and 1.81 times that of RM, RM-PB, and Ni PBA, respectively. It was found that 1 O 2 was the main reactive oxygen species (ROS) dominated the degradation process, and its formation was accompanied by the mutual conversion of Ni(II)/Fe(II) and Ni(III)/Fe(III). Notably, the degradation process maintained a satisfactory efficiency over a wide pH range (3–9) and exhibited strong anti-interference ability against impurities such as Cl − , SO 4 2− , and NO 3 − . The components and contents of RM-Ni PBA remained relatively stable during the degradation process. In addition, the degradation intermediates of CIP were identified, and possible degradation pathways were proposed. This study is expected to provide theoretical basis and technical guidance for the application of RM-based heterogeneous catalyst in the treatment of antibiotic wastewater.
研究领域:
环境科学
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材料科学
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废水处理
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DOI
PubMed
ACS Nano
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2025
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IF 16
Ruoxuan Sun,Minghui Zhu,Jie Chen,Lei Yan,Liyi Bai,Jiqiang Ning,Yijun Zhong,Yong Hu
The electrochemical synthesis of hydrogen peroxide (H2O2) via the two-electron oxygen reduction reaction (2e– ORR) is a promising alternative to the conventional anthraquinone method. However, due to local alkalinization near the catalyst surface, the restricted oxygen replenishment and insufficient activated water molecule supply limit the formation of the key *OOH intermediate. Herein, a pulsed electrocatalysis approach based on a structurally optimized S/N/O tridoped hollow carbon bowl catalyst has been proposed to overcome this challenge. In an H-type electrolytic cell, the pulsed method achieves a superior H2O2 yield rate of 55.6 mg h–1 mgcat.–1, approximately 1.6 times higher than the conventional potentiostatic method (34.2 mg h–1 mgcat.–1), while maintaining the Faradaic efficiency above 94.6%. In situ characterizations, finite element simulations, and density functional theory analyses unveil that the application of pulsed potentials mitigates the local OH– concentration, enhances the water activation and proton generation, and facilitates oxygen production within the hollow bowl-like carbon structure. These effects synergistically accelerate the formation kinetics of the *OOH intermediate by the efficient generation of *O2 and *H2O intermediates, leading to superior H2O2 yields. This work develops a strategy to tune catalytic environments for diverse catalytic applications.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jing Zhang,Dumeijin Gong,Zian Cheng,Chao Shan
The peroxone (O 3 /H 2 O 2 ) process has long suffered from inefficient performance for water decontamination at acidic pHs. Herein, we find the evident capability of trace Ce(III) to boost the acidic peroxone process. In contrast to the negligible degradation (∼6% in 60 min) of oxalic acid (OA) as a recalcitrant compound in the O 3 /H 2 O 2 system, efficient removal of OA (∼95 %) was achieved by introducing trace Ce(III) (0.30 µM). OA was identified as an effective ligand activating Ce(III) by forming the Ce(III)-OA complex, which served as the catalytic active component to accelerate the decomposition of O 3 and H 2 O 2 to produce •OH and promote the co-degradation of refractory pollutant atrazine and ibuprofen. The remarkable catalytic activity of trace Ce(III) for peroxone reaction resulted from the efficient interconversion of Ce(III/IV) relying on both the favorable electron transfer from the ternary Ce(III)-OA-hydroperoxo complex to O 3 and the rapid reduction of Ce(IV) back to Ce(III) mainly by H 2 O 2 . Furthermore, the catalytic performance of Ce(III) for peroxone process outperformed Fe(II), Cu(II), and Co(II). This study puts forward an effective method to extrapolate the applicability of the peroxone (O 3 /H 2 O 2 ) process to the acidic range and enlightens the development of Ce-catalyzed peroxone processes.
研究领域:
环境科学
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化学
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Jiawei Hu,Jiaming Li,Zhongyi Pu,Wen Xiao,Huan Yu,Zhihao Zhang,Fang Yu,Chao Liu,Qinfang Zhang
Heterostructured visible-light-responsive photocatalysts represent a prospective approach to achieve efficient solar-to-chemical energy conversion. Herein, we propose a facile self-assembly technique to synthesize NiO nanoparticles/C 3 N 5 nanosheets (NOCN) heterojunctions for hydrogen (H 2 ) evolution catalysis and hydrogen peroxide (H 2 O 2 ) production under visible light. In this regard, the black NiO nanoparticles (NPs) were tightly anchored on the surface of C 3 N 5 nanosheets (CNNS) to construct S-scheme NOCN heterojunction, enabling efficient charge separation and high redox capability. Obtained results elucidated that the incorporated NiO NPs significantly promote light-harvesting efficiency and photo-to-thermal capacity over the NOCN composites. The enhanced photothermal effect facilitates the charge carrier transfer rate across the heterojunction and boosts the surface reaction kinetics. Accordingly, the photocatalytic performances of CNNS for H 2 release and H 2 O 2 production can be manipulated by introducing NiO NPs. The modified photocatalytic properties of NOCN composites are ascribed to the synergistic effects of all integrated components and the S-scheme heterojunction formation. Impressively, the high H 2 evolution photocatalysis efficiency of NOCN nano-catalysts in seawater certifies their potential environmental applicability. Among all, the 12-NOCN nano-catalyst exhibits a higher photocatalytic efficiency for H 2 release (112.2 μmol∙g −1 ∙h −1 ) and H 2 O 2 production (91.2 μmol∙L −1 ∙h −1 ). Besides, the 12-NOCN nano-catalyst reveals excellent recyclability and structural stability. Additionally, the possible mechanism for photothermal-assisted photocatalysis is proposed. This work affords a feasible pathway to design photothermal-assisted S-scheme heterojunctions for diverse photocatalytic applications.
研究领域:
光催化
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材料科学
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环境科学
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化学工程
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DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Lingzheng Feng,Wei Han,Xiaojun Guo,Jianzhang Zhu,Jiaqi Shen,Xingguo Xiao,Hudong Yan,Fei Zha,Haifeng Tian,Xiaohua Tang
Nitrogen doping introduces sulfur vacancies and lattice distortion into In 2 S 3 , which enhances charge separation and provides anchoring sites for Ag species. • Achieves a high H 2 O 2 production rate of 965 μmol g −1 ·h −1 via the 2e − ORR pathway. • DFT reveals Ag single atoms optimize *OOH adsorption; clusters boost electron redistribution. • Exhibits efficient degradation of perphenazine (95% removal within 30 min). • Operates effectively in pure water without sacrificial agents and shows excellent stability. To address the rapid recombination of photogenerated charge carriers in indium sulfide (In 2 S 3 ) and meet the growing demand for efficient photocatalytic hydrogen peroxide (H 2 O 2 ) production systems, this study proposes a rational design. Leveraging active nitrogen species generated from urea decomposition during hydrothermal treatment, we successfully doped the In 2 S 3 lattice to construct a nitrogen-modified indium sulfide (N-In 2 S 3 ) substrate, and subsequently co-anchored silver single atoms and clusters (Ag SA+C /N-In 2 S 3 ) onto it for efficient photocatalytic H 2 O 2 production and pollutant degradation. Nitrogen (N) doping induced sulfur vacancies and lattice distortion, enhancing charge separation and surface reactivity. Ag species were atomically dispersed and firmly anchored onto the N-In 2 S 3 support, serving as efficient electron sinks and active sites. The optimized Ag SA+C /N-In 2 S 3 achieved a remarkable H 2 O 2 production rate of 965 μmol g −1 h −1 in pure water via a predominant two-electron oxygen reduction reaction (2e − ORR) pathway, significantly outperforming pristine In 2 S 3 and N-In 2 S 3 . Combined with experimental characterization and DFT calculations revealed that Ag single atoms optimized the adsorption of the *OOH intermediate and reduced the reaction free energy barrier, while Ag clusters facilitated electron redistribution and enhanced oxygen activation. It also demonstrated superior photocatalytic degradation efficiency for organic pollutant like perphenazine (95% removal in 30 min). This study highlights the synergistic effect of bulk doping and surface atomic-level engineering in developing high-performance photocatalysts for sustainable chemical synthesis and environmental remediation. Download: Download high-res image (140KB) Download: Download full-size image
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高影响因子
MOLECULAR AND CELLULAR BIOCHEMISTRY
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2026
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IF 4.7
Liu Xiang,Sun Jing-Jing,Mao Chang-Kun,Cao Yong-Sheng,Deng Qi-Fei,Li Guang-Yuan
Cryptorchidism, characterized by the failure of one or both testes to descend into the scrotum, is the most prevalent urogenital malformation in male infants and an important risk element of male infertility and testicular cancer. The purpose of this study was to investigate the molecular mechanisms underlying cryptorchidism-induced testicular damage, with a focus on the role of USP35. Here we established a unilateral experimental cryptorchidism model of Sprague-Dawley rats by resetting the left testis to the abdominal cavity and suturing the inguinal canal, thus preventing its natural descent. The findings indicated that apoptosis and oxidative stress (OS) levels were increased in the undescended testis (UDT) compared to the descended testis (DT) group. Subsequent mRNA sequencing of DT and UDT tissues revealed that ubiquitin specific peptidase 35 (USP35) expression was downregulated in the UDT, implying that USP35 may be an important factor in the pathogenesis of cryptorchidism. To further investigate, an oxidative damage model was constructed using H 2 O 2 -treated GC-1 spermatogonia. USP35 expression was reduced in H 2 O 2 -exposed cells, while overexpression of USP35 attenuated H 2 O 2 -induced oxidative damage by inhibiting apoptosis and OS. Mechanistically, USP35 interacted with nuclear factor erythroid 2-related factor 2 (NRF2) and stabilized its protein expression via deubiquitination. Impairment of NRF2 function abolished the protective effect of USP35 against oxidative damage in H 2 O 2 -treated GC-1 spermatogonia. Overall, these results highlight the significance of the USP35-NRF2 axis in protecting spermatogonia from oxidative injury, suggesting that USP35 may be a potential therapeutic target against cryptorchidism-induced early germ cell damage.
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高影响因子
INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
·
2026
·
IF 4.7
Shuai Liu,Yuzhe Liu,Yuan Sun,Yalei Han,Mingjun He,Junjie Tang,Wei Jiang
Single crystal superalloy scrap represents an important secondary resource containing rhenium (Re), yet only a very small fraction of high-purity scrap can be directly reused as remelting feedstock, while most of the material must undergo hydrometallurgical processing to enable Re recovery. In hydrometallurgical processes, the formation of oxide-dominated barrier layers hinders effective dissolution. To address this, an electrochemical leaching method using a mixed electrolyte of HCl and H 2 O 2 was developed. The process parameters were optimized to 3 mol·L −1 HCl, 9% ( v /v) H 2 O 2 , a current density of 0.36 A·cm −2 , and an electrolysis time of 2 h. Under these conditions, the current efficiency reached 77% and the Re leaching efficiency was 97.9%. The barrier layers consisted of a chloride deposit layer, a Ta W oxide layer, and a Cr-rich oxide layer. These layers were effectively broken down during the electrochemical process. Specifically, the Ta W oxide layer underwent cracking and spallation, while the Cr-rich oxide layer was progressively destabilized and dissolved under the coupled chemical and electrochemical effects. This method successfully disrupted the oxide barrier layers and significantly enhances Re leaching efficiency. It provides an efficient nitric-acid-free route for recovering Re from single crystal superalloy scrap.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Peng Lin,Yujie Li,Jun Wang,Shengjian Lin,Junheng Huang,Zhenhai Wen
While noble metal-based catalysts remain the most effective for the four-electron oxygen reduction reaction (ORR), nitrogen-doped carbon materials are promising non-metal alternatives. However, atomic-level modulation of pyridinic-N sites to rival Pt-based ORR activity remains a fundamental challenge. To address this, we developed a novel “defect-guided in situ atomic substitution” strategy. Using highly fluorinated graphene as a precursor, we achieved synchronous defluorination, graphitization, and precise nitrogen doping through a one-step thermochemical process. C F bond cleavage generates transient carbon vacancies that serve as anchoring sites, constructing a catalytic surface rich in pyridinic nitrogen. The resulting nitrogen-doped graphene catalyst (PN-G) exhibits outstanding bifunctional activity: for ORR, it achieves a half-wave potential of 0.86 V and an average electron transfer number of ∼3.90; for the hydrogen peroxide oxidation reaction (HPOR), its onset potential is reduced by over 0.5 V compared to the oxygen evolution reaction (OER). In situ Raman identified *O 2 − as a central role in bidirectional oxygen electrocatalysis (ORR and HPOR). Utilizing PN-G catalyst, we constructed a rechargeable zinc‑oxygen battery employing an H 2 O 2 -mediated electrolyte. This battery delivers a peak power density of 710 mW cm −2 and a round-trip energy efficiency of ∼96% at 5 mA cm −2 . This work not only establishes a controllable synthetic route for high-performance metal-free carbon catalysts but also provides a practical approach for designing efficient metal-air batteries.
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PubMed
高影响因子
TALANTA
·
2026
·
IF 6.7
Yu Pan,Amin Zhang,Chengliang Qi,Yueming Wang,Xin Chen,Wenli Wang,Xichang Wang,Yuan Liu
In-situ pore-confined growth of ultra-small Pt nanoclusters within mesoporous SiO 2 . • Au-Pt@SiO 2 nanozyme exhibits superior peroxidase-like activity with K m of 6.077 mM. • Enzyme-free electrochemical biosensor achieves 0.3 μM LOD. • Exceptional long-term stability retaining >85% activity after 30 days of storage. • Real-time quantitative profiling of single cancer cell H 2 O 2 efflux upon PMA trigger. Accurate quantification of H 2 O 2 released by tumor cells is important for characterizing cancer-associated oxidative stress, yet conventional biosensors often face an intrinsic trade-off between catalytic activity and structural stability. Herein, we present a rational strategy for real-time electrochemical monitoring of cancer-associated oxidative stress species through the in-situ fabrication of ultrasmall Pt nanozymes confined within the mesoporous silica shell of gold bipyramids (AuPt@SiO 2 ). In this architecture, the Au core provides conductive nucleation and anchoring sites, the mesoporous SiO 2 shell regulates Pt growth and affords structural stabilization and molecular-sieving protection, and Pt serves as the catalytic center for H 2 O 2 reduction. The resulting AuPt@SiO 2 nanozyme exhibited pronounced peroxidase-like activity with a favorable Michaelis-Menten constant (K m ) of 6.08 mM toward H 2 O 2 . After integration into a Nafion-based sensing interface, the enzyme-free sensor provided complementary linear ranges of 0.25-60 mM by cyclic voltammetry and 1-2100 μM by amperometry with a detection limit at 0.3 μM of H 2 O 2 . The electrochemical sensor based on AuPt@SiO 2 also demonstrated excellent repeatability and exceptional stability, retaining over 85% of its initial response after 30 days. Importantly, this platform enabled label-free monitoring of phorbol 12-myristate 13-acetate (PMA)-triggered H 2 O 2 efflux from MGC-803 gastric cancer cells and differentiated their oxidative-stress phenotype from that of normal gastric epithelial cells. The apparent H 2 O 2 -equivalent response normalized to cell number was approximately 1.72 × 10 −13 M per cell. This work highlights the potential of confined nanozymes for high-performance H 2 O 2 sensing and precise pathological profiling at the single-cell level. Download: Download high-res image (405KB) Download: Download full-size image
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高影响因子
危险品化学品经营许可证（带存储）