ELECTROCHIMICA ACTA
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2026
·
IF 5.8
Jinxin Xie,Yujue Wang,Haisong Li,Yinqiao Zhang,Minghua Zhou
The mass transfer of O 2 /O 3 was improved at three-phase interface of CB‑PTFE. • CB enabled the synergistic reduction of O 2 /O 3 for •OH generation. • O 3 reduction and catalytic ozonation accelerated phenol mineralization. • Phenol removal and mineralization were 100% and 85% in ten-cycles. The electro-peroxone (E-peroxone) process suffered from the limited mass transfer and insufficient utilization of gaseous O 2 /O 3 mixture. Herein, a hydrophobic carbon black‑polytetrafluoroethylene (CB‑PTFE) electrode was fabricated to construct a gas‑liquid‑solid three-phase interface for improving phenol mineralization. The CB-PTFE electrode exhibited a high contact angle of 143.3°, which enhanced the mass transfer of O 2 /O 3 effectively. Compared with the hydrophilic carbon black‑polyvinylidene fluoride (CB‑PVDF) cathode (72.9°, 51.8%), CB‑PTFE achieved 86.0% TOC removal (0.016 min −1 ) at 120 min in E-peroxone, significantly outperforming sole ozonation (O 3 , 40.0%, 0.004 min −1 ) and electro‑oxidation (EO, 7.2%, 0.004 min −1 ). The greater TOC removal in CB-PTFE/O 3 (66.3%, 0.0095 min −1 ) than that in O 3 indicated that CB-PTFE had catalytic ozonation activity. Electrochemical analysis by a rotating ring‑disk electrode (RRDE) revealed that CB enabled simultaneous 2‑electron oxygen reduction reaction (ORR) to H 2 O 2 (n = 2.23) and efficient 1‑electron O 3 electro‑reduction for increased cathodic current and hydroxyl radical (•OH) generation under the O 2 /O 3 atmosphere. The highest •OH yield (280.5 μmol/L) was obtained using hydrophobic CB-PTFE in E‑peroxone, and theoptimal conditions were the applied current of 20 mA, in‑gas O 3 concentration of 50 mg/L and neutral pH of 7.0. Furthermore, the hydrophobic CB‑PTFE electrode maintained nearly 86.0% TOC removal over ten-cycles with stable structural integrity, despite a slight decrease of hydrophobicity. The reduction of O 2 /O 3 , catalytic ozonation and peroxone reaction were coupled in E-peroxone synergistically, which offered a promising strategy for efficient pollutant abatement. Download: Download high-res image (262KB) Download: Download full-size image
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CHEMICAL ENGINEERING JOURNAL
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2025
·
IF 13.2
Chen Wang,Yunpeng Zou,Xiaohui Wu,Xiangling Zhang,Wenjiao Sang,Tao Zhou,Mingjie Huang
Realizing efficiently sustainable generation of singlet oxygen ( 1 O 2 ) in the O 2 activation-based systems is crucial, since 1 O 2 can oxidize many organic pollutants via a non-radical pathway that is preferable in complex water matrices e.g. saline wastewaters. In this study, a boosted strategy that introduced oxygen vacancies (OVs) and surface carboxyl groups (−COOH) onto electron-rich copper‑iron oxides, was proposed by a facile mechanochemical ball-milling process with citrate ligands (Cit). Notably, the resulting Cit@CuFe 2.5 O x catalyst enabled efficient O 2 activation via a selective non-radical pathway, achieving a standardized pseudo-first-order rate constant ( k obs ) of 0.073 min −1 ·g −1 for sulfamethoxazole (SMX) degradation, with over 90 % of the oxidative contribution attributed to 1 O 2 . The ball-milling procedure with Cit could cause the generation of abundant OVs for O 2 adsorption and activation . Mechanistic analysis and theoretical calculations revealed that the OVs accelerated electron transfer from adjacent Cu(I) atoms to adsorbed O 2, facilitating the generation of O 2 − and markedly lowering the free energy barrier for its subsequent conversion to 1 O 2 other than H 2 O 2 . Additionally, the surface-bound −COOH groups facilitated the transformation of molecular O 2 to adsorbed O 2 at OVs sites, further lowering the thermodynamic barrier of the O 2 ⟶ O 2 − ⟶ 1 O 2 pathway. This study provides a simple and cost-effective promotional strategy for O 2 activation by ball-milled electron-rich materials, offering an easily obtained method to induce 1 O 2 -dominated oxidation of recalcitrant organic pollutants in the treatment of high-salinity wastewater.
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INTERNATIONAL JOURNAL OF ENERGY RESEARCH
·
2022
·Vol. 46
·期 14
·19357-19367
·
IF 4.672
Jiuqing Liu,Feifei Song,Junying He,Zikun Hong,Qihou Li,Ya Chen,Lishun Bai,Fanli Zeng,Chen Cheng,Zehao Chen
Summary Owing to its unparalleled theoretical energy density, the Li-O 2 batteries are thought to be one of the most promising energy storage systems, but its application is seriously hindered by its potential safety risks arising from the passivation and corrosion of lithium anode. To address these issues, it is an efficient way to develop functionalized separator that could prevent the migration of anions and macromolecules from cathode toward anode. Herein, a novel Nafion-functionalized polyethersulfone (PES)-based ion-permselective separator was prepared by using non-solvent induced phase separation (NIPS) method. The Nafion ensures a better physical strength of the composite separator, and further characterizations show that the obtained composite separator owns good ionic conductivity (0.52 mS cm −1 ), high lithium ion migration number (0.80), and better cyclic stability (120 cycles, 1000 mAh g −1 ). Consequently, the composite separator serves as an excellent candidate to solve the “shuttle effect” of redox mediators (RMs), the assembled Li-O 2 battery with composite separator adding LiI as RMs presents lower charge overpotential and longer cycle stability (170 cycles, 1000 mAh g −1 ).
研究领域:
材料科学
·
电化学
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yongcen Chen,Xuemin Ma,Yajuan Hu,Huiyue Wang,Peirong Zhou,Xiaoping Tian,Haofeng Wang,Yun He,Gang Tao,Rui Cai,Junliang Chen
Diabetic wounds are marked by persistent infection, hypoxia, excessive reactive oxygen species (ROS), and impaired angiogenesis, which present significant challenges for clinical management. In this study, a pH/ROS dual-responsive multifunctional hydrogel (QOF-EGCG/Hb@PDA) was constructed by grafting 3-carboxyl-4-ffuorophenylboronic acid (FPBA) onto Quaternary ammonium chitosan (QCS) to form Schiff base bonds with Oxidized gellan gum (OGG) (pH response), and by reacting FPBA with Epigallocatechin gallate (EGCG) to form borate bonds (ROS response). Hb@PDA nanoparticles were then loaded into the hydrogel. Under acidic conditions, the cleavage of Schiff base bonds triggers the release of Hb@PDA, providing sustained oxygen delivery to alleviate hypoxia. Additionally, in ROS-rich environments, the cleavage of borate ester bonds promotes EGCG release, exerting antioxidant and anti-inflammatory effects. QOF-EGCG/Hb@PDA displays excellent self-healing capacity and tissue adhesion, as well as remarkable photothermal activity. Furthermore, it demonstrates excellent antibacterial, antioxidant, anti-inflammatory, pro-angiogenic, and hemostatic properties. In vivo studies confirmed that this hydrogel markedly accelerated diabetic wound healing by enhancing epithelial regeneration, promoting collagen deposition, regulating inflammatory responses, and facilitating angiogenesis. Transcriptomic analysis revealed that the hydrogel promotes angiogenesis by activating the HIF-1α/VEGF signaling pathway, which plays a pivotal role in vascular formation and tissue regeneration, thereby accelerating the healing of diabetic wounds. Collectively, QOF-EGCG/Hb@PDA provides a promising and comprehensive strategy with great potential for application in diabetic wound treatment.
研究领域:
生物医学工程
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伤口愈合
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药物递送
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纳米医学
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组织工程
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免疫调节
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再生医学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yixuan Wen,Qizhen He,Shuaijun Ding,Wei Zhou,Lei Deng,Liqiang Zhang,Tongde Shen,Qingxiang Yang,Peng Jia,Yuqing Qiao
Silver (Ag) plays an important role as a cathode catalyst in lithium-oxygen batteries (Li-O 2 batteries). However, the catalytic mechanism of Ag remains unclear. Despite efforts dedicated to studying interfacial reactions, observing efficient reactions and ion transport at the Ag-Li solid–solid interface continues to be a challenge. Here, we used Ag nanowires (Ag NWs) as working electrodes, creating a lithiation-oxidation microenvironment within spherical aberration-corrected transmission electron microscopy (ETEM) through a two-step method to investigate the reaction mechanisms at the Ag-Li interface. The lithiation process generates Ag 3 Li 10 , while the oxidation process precipitates Ag nanoparticles (Ag NPs). The alternating reactions of Ag-Ag 3 Li 10 -Ag form a cycle process, elucidating the transport pathway of Li + at the Ag-Li solid–solid interface during discharge process and demonstrating a typical lithium pump effect. Density Functional Theory (DFT) calculations also confirm these results. This work provides novel insights into the interfacial mechanisms of Ag catalysts in Li-O 2 batteries, offering valuable guidance for strategies to monitor and control complex, multi-step interfacial reactions.
研究领域:
电化学
·
材料科学
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储能技术
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纳米材料
·
原位表征
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Lei Chen,Wenxia Zhuang,Jingmin Lan,Xiaoling Liu,Shi Jiang,Lei Wang,Yu Zhou,Jun Wang
Mg-bearing MTW silicalite zeolite, MgSi-ZSM-12, was straightforwardly synthesized by involving an unusual acidic pre-gelation system and engaged as the task-specific support for loading the Au nanoparticles (NPs). The resulting Au/MgSi-ZSM-12 catalyst showed stably excellent activity for the oxidation of HMF into FDCA in the presence of atmospheric dioxygen (O 2 ) without externally adding any liquid base, affording a yield of 87 % and turnover number (TON) of 331 based on the surface Au sites. Superior basicity was evidenced by embedding Mg species into the all-silica zeolitic skeleton, which enables strong, weak, and near-zero affinity towards aldehyde, alcohol, and carboxyl groups, respectively, thus, allows rapid and high-uptake adsorption of HMF, but negligible adsorption of FDCA. This unique feature of the Mg-bearing all-silica zeolite support together with its synergy with the active sites of Au NPs is revealed to accelerate the production of FDCA under the base-free mild condition.
研究领域:
催化化学
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材料科学
·
环境化学
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JOURNAL OF POWER SOURCES
·
2020
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IF 8.247
Hongying Tang,Kang Geng,Jinkai Hao,Xiaojuan Zhang,Zhigang Shao,Nanwen Li
Quaternized poly(sulfone)s based on trimethylamine (PSf-TMA-x) and triethylamine (PSf-TEA-x) are developed to form quaternary ammonium (QA)-biphosphate ion pairs as promising high temperature proton exchange membrane (HT-PEM) in H 2 /O 2 fuel cells. The strong QA-biphosphate ion-pair interaction results in high acid absorption and thus high proton conductivity of 78.1 mS cm −1 for PSf-TEA-110/PA membrane at 160 °C in spite of its lower degree of functionalization. Thus, the peak power density of more than 400 mW cm −2 is achieved at 160 °C for the quaternized PSf membranes in H 2 /O 2 fuel cell, which is higher than that of the poly(benzeimidazole) ( m -PBI) membrane (370 mW cm −2 ). Subsequently, the degradation mechanism of the PSf membranes is demonstrated using NMR technique to be occurred in both the polymer backbone and the QA groups. The stability investigation of model compounds further confirms that the degradation of the membranes resulted from the scission of ether linkage and isopropylidene group and the SN2 nucleophilic substitution of QA at operating conditions. Therefore, the significant performance decrease is observed and the lifetime is only less than 30 h at 200 mA cm −2 which is much lower than that of m -PBI membrane (>40 h).
研究领域:
材料科学
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化学工程
·
能源科学
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Advanced Healthcare Materials
·
2023
·Vol. 12
·期 15
·2202280
·
IF 10
Wenya Li,Rongtian Li,Qiang Ye,Yiming Zou,Xing Lu,Wenhua Zhang,Jinxiang Chen,Yinghua Zhao
Nanomedicine exhibits emerging potentials to deliver advanced therapeutic strategies in the fight against triple-negative breast cancer (TNBC). Nevertheless, it is still difficult to develop a precise codelivery system that integrates highly effective photosensitizers, low toxicity, and hydrophobicity. In this study, PCN-224 is selected as the carrier to enable effective cancer therapy through light-activated reactive oxygen species (ROS) formation, and the PCN-224@Mn 3 O 4 @HA is created in a simple one-step process by coating Mn 3 O 4 nanoshells on the PCN-224 template, which can then be used as an “ROS activator” to exert catalase- and glutathione peroxidase-like activities to alleviate tumor hypoxia while reducing tumor reducibility, leading to improved photodynamic therapeutic (PDT) effect of PCN-224. Meanwhile, Mn 2+ produced cytotoxic hydroxyl radicals (∙OH) via the Fenton-like reaction, thus producing a promising spontaneous chemodynamic therapeutic (CDT) effect. Importantly, by remodeling the tumor microenvironment (TME), Mn 3 O 4 nanoshells downregulated hypoxia-inducible factor 1 α expression, inhibiting tumor growth and preventing tumor revival. Thus, the developed nanoshells, via light-controlled ROS formation and multimodality imaging abilities, can effectively inhibit tumor proliferation through synergistic PDT/CDT, and prevent tumor resurgence by remodeling TME.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Junjie Wu,Peng Shen,Xian Qin,Yulu Yang,Chuanchuan Lin,Xuan Li,Wenbo Geng,Pengfei Gao,Lixue Chen,Li Miao,Yang Jiao,Bailong Tao
Bacterial wound infection is a major challenge to human health worldwide. In this study, a composite nanogenerator, CaO 2 @ZIF-67-PLL, was fabricated via a bottom-up approach with chemodynamic therapy (CDT)/hypoxia improvement for rapid therapy of biofilm-infected wounds. Under a pathologically acidic microenvironment, the out layer ZIF-67 can be decomposed to rapidly release Co 2+ and CaO 2 ; Subsequently, the unprotected CaO 2 reacts with H 2 O to produce O 2 and H 2 O 2 . The self-supply of O 2 relieves hypoxia and inflammatory response induced by infections, while the generated H 2 O 2 and poly- l -lysine (PLL) exhibited synergistic strong anti-biofilm capability against Escherichia coli ( E. coli) and Staphylococcus aureus (S. aureus) as assessed by reactive oxygen species (ROS) generation, membrane permeability change, ATP reduction, o -nitrophenyl-β-d-galactopyranoside (ONPG) hydrolysis and intracellular component leakage. Meanwhile, CaO 2 @ZIF-67-PLL exhibited good cytocompatibility and promoted the adhesion, proliferation, and migration of NIH-3T3 cells by enhancing the expression of wound healing-related genes (TGF-β1, VEGF, α-SMA, Col I, Col III, and Wnt-5a). Notably, CaO 2 @ZIF-67-PLL could significantly improve the healing process of S. aureus -infected wounds via suppressed inflammatory responses, enhanced collagen disposition and angiogenesis, and stimulated HIF-1α, CD31, and Wnt-5a/β-Catenin signaling pathways. These results indicated the potential of CaO 2 @ZIF-67-PLL nanogenerator for clinical application in infected wound treatment.
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JOURNAL OF MEMBRANE SCIENCE
·
2022
·
IF 10.53
Xiaohong Zou,Qian Lu,Cuie Wang,Sixuan She,Kaiming Liao,Ran Ran,Wei Zhou,Liang An,Zongping Shao
Before the practical application of the Li–O 2 battery (LOB), a critical issue regarding large overpotential upon charging (which causes irreversible side reactions and low energy efficiency) should be resolved. The utilization of redox mediators (RMs) which oxidatively decompose insulating discharge product, Li 2 O 2 , is one promising solution to address this issue. However, the soluble RMs can easily diffuse to and react with the Li metal anode (encountering Li dendrites is even worse). Here, a chemical self-assembly strategy is introduced into the fabrication of the iodide-redox-phobic and Li-ion-philic membrane for LOBs, in which the electronegative δ-MnO 2 layer is in-situ grown on commercial polyethylene (PE) membrane (MnO 2 @PE). The electronegative MnO 2 layer can simultaneously repel the shuttle of iodide species and regulate the uniform Li + deposition. Controlling cut-off capacity of 1000 mAh g −1 , iodide-redox-based LOB with MnO 2 @PE demonstrates low overpotentials (∼0.7 V vs. Li + /Li), dendrite-suppressing capability, as well as impressive long-term reversibility over 500 cycles (2000 h), which urges the LOB technology competitive among the next-generation rechargeable power systems.
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Theranostics
·
2022
·
IF 11.6
Qiqi Xu,Yuetong Zhang,Zulu Yang,Guohui Jiang,Mingzhu Lv,Huan Wang,Chenghui Liu,Jiani Xie,Chengyan Wang,Kun Guo,Zhanjun Gu,Yuan Yong
Nanozyme-based tumor collaborative catalytic therapy has attracted a great deal of attention in recent years. However, their cooperative outcome remains a great challenge due to the unique characteristics of tumor microenvironment (TME), such as insufficient endogenous hydrogen peroxide (H 2 O 2 ) level, hypoxia, and overexpressed intracellular glutathione (GSH). Methods: Herein, a TME-activated atomic-level engineered PtN 4 C single-atom nanozyme (PtN 4 C-SAzyme) is fabricated to induce the “butterfly effect” of reactive oxygen species (ROS) through facilitating intracellular H 2 O 2 cycle accumulation and GSH deprivation as well as X-ray deposition for ROS-involving CDT and O 2 -dependent chemoradiotherapy. Results: In the paradigm, the SAzyme could boost substantial ∙OH generation by their admirable peroxidase-like activity as well as X-ray deposition capacity. Simultaneously, O 2 self-sufficiency, GSH elimination and elevated Pt 2+ release can be achieved through the self-cyclic valence alteration of Pt (IV) and Pt (II) for alleviating tumor hypoxia, overwhelming the anti-oxidation defense effect and overcoming drug-resistance. More importantly, the PtN 4 C-SAzyme could also convert O 2 ·- into H 2 O 2 by their superior superoxide dismutase-like activity and achieve the sustainable replenishment of endogenous H 2 O 2 , and H 2 O 2 can further react with the PtN 4 C-SAzyme for realizing the cyclic accumulation of ∙OH and O 2 at tumor site, thereby generating a “key” to unlock the multi enzymes-like properties of SAzymes for tumor-specific self-reinforcing CDT and chemoradiotherapy. Conclusions: This work not only provides a promising TME-activated SAzyme-based paradigm with H 2 O 2 self-supplement and O 2 -evolving capacity for intensive CDT and chemoradiotherapy but also opens new horizons for the construction and tumor catalytic therapy of other SAzymes.
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高影响因子
ELECTROCHIMICA ACTA
·
2022
·
IF 7.336
Jie Li,Youcai Lu,Shiyu Ma,Zhongjun Li,Qingchao Liu
Li–O 2 battery has attracted wide attention because it can satisfy the need for a new energy storage system with high energy density. However, poor oxygen reduction (ORR)/oxygen evolution (OER) kinetics involving Li 2 O 2 formation/decomposition is a major obstacle to its development. By designing suitable cathode with desired structure and surface electronic states, the formation/morphology of Li 2 O 2 and the reaction kinetics of charge process can be efficiently optimized simultaneously. In this work, a novel sulfur (S) and chlorine (Cl) co-doped porous carbon (CSC) were synthesized by one-step pyrolysis strategy, and the amount of heterogeneous atoms could be flexibly controlled by different calcination temperatures . Experimental combined with theoretical calculations show that the content of C Cl bond plays an important role in the adsorption of intermediate LiO 2 , thus regulating the morphology of Li 2 O 2 and ultimately affecting the release of battery energy. The C S bond mainly acts on the dynamics of the ORR and OER processes, which has an important influence on improving the round-trip efficiency of the battery. Benefiting from the synergistic effect of heteroatoms , the electrochemical performances of the Li–O 2 battery, including round-trip efficiency, discharge capacity and cycling stability are greatly improved.
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