ACS Earth and Space Chemistry
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2023
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IF 3.4
Hao Tian,Xue-Bin Zhang,Yin-Ping Li,Qing He,Na-Na Tian,Song-Hai Wu,Xu Han
Although inorganic Fe(IV)═O oxo and Fe(III)-OOH peroxo have attracted more attention in aqueous environments, direct evidence for the characterization and identification of those oxidizing species is still lacking. In this study, the doped Cu/Co increases the reactivity of ferrihydrite/hematite in oxidizing As(III) by S(IV)-O2 under alkaline and dark conditions. Quenching experiments exclude the contributions of ·OH, O2•–, SO3•–, SO4•–, SO5•–, HSO5–, and H2O2 and confirm that peroxo and oxo are primary oxidizing species in As(III) oxidation. Electrochemical analyses indicate that Fe(IV)═O oxo and Fe(III)-OOH peroxo are primarily located on the surface of ferrihydrite and hematite. Selective oxidation of methyl phenyl sulfoxide and methyl phenyl sulfide to the corresponding oxidation products further reveals the presence of ≡Fe(IV)═O oxo on both ferrihydrite and hematite, and the doped Cu/Co significantly decreases the produced ≡Fe(IV)═O oxo on ferrihydrite, while increases the produced ≡Fe(IV)═O oxo on hematite. Meanwhile, selective oxidation of benzyl alcohol to benzaldehyde indicates the presence of ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite, and the doped Cu/Co apparently increases the produced ≡Fe(III)-OOH peroxo on ferrihydrite and hematite. Raman analysis further reveals the presence of ≡Fe(IV)═O oxo and ≡Fe(III)-OOH peroxo on pure and metal-doped ferrihydrite/hematite, which also confirms that the doped Cu/Co decreases the produced ≡Fe(IV)═O oxo on ferrihydrite and increases ≡Fe(IV)═O oxo on hematite, while apparently increasing ≡Fe(III)-OOH peroxo on both ferrihydrite and hematite. This study enriches our understanding on the oxidizing species in the S(IV)-mediated oxidation processes under alkaline conditions, providing new insight on the oxidation reactivity of surface peroxo and oxo species mediated by the doped metal ions.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2021
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IF 2.495
Qian-Qian Huang
A novel tetranuclear nickel(II)-flavonolate complex [Ni II 4 (fla) 4 (CH 3 O) 4 (H 2 O) 4 ] (flaH: 3-Hydroxyflavone, flavonol) was synthesized. Its crystal structure and spectroscopic features have been investigated in details by physicochemical methods and single crystal X-ray diffraction. Different from other mononuclear metal-flavonolate complexes, this complex demonstrates a cluster molecular structure which has four Ni II centers, and each Ni II centre is coordinated by a bidentate flavonolate, three methanol and a water molecule. The crystal of this complex is tetragonal crystal system: space group I 41/a, a = 24.4361(14), b = 24.4361(14), c = 12.7972 (14), α = β = γ = 90 ° , V = 7641.5 (12), Z = 4. The complex can react with O 2 , in other words, it has enzymatic reactivity just like enzyme-substrate model of quercetin 2,3-dioxygenase, and the reaction products are similar with the other reported enzyme-substrate models.
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Acta Biomaterialia
·
2022
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IF 10.633
Furong Liu,Tao He,Songlin Gong,Meiling Shen,Shuang Ma,Xianzhou Huang,Lu Li,Li Wang,Qinjie Wu,Changyang Gong
Combining the internal force-driven chemodynamic therapy (CDT) and the external energy-triggered photodynamic therapy (PDT) holds great promise to achieve an advanced anticancer effect based on reactive oxygen species (ROS). However, the insufficient oxy-substrates supply in tumor microenvironment, like hydrogen peroxide (H 2 O 2 ) and oxygen (O 2 ), is the Achilles heel that greatly restricts the efficacy of this ROS-based treatment. Herein, the construction of a c opper p e roxide-based tumor pH-re s ponsive a utocatalytic nano r eactor (CESAR), via an albumin-mediated biomimetic mineralization strategy is described. The decoration of human serum albumin endows the nanoreactor good hydrophilicity and biocompatibility, which is highly desired for the metal-based materials. Upon exposure to acidic tumor microenvironment, CESAR presents a pH-triggered disintegration with Cu 2+ , H 2 O 2 and O 2 generated instantly. The generated H 2 O 2 complements the hyperoxide deficiency and initiates a localized Fenton-like reaction with the assistance of Cu 2+ for highly toxic hydroxyl radicals (•OH) production for improving CDT. The evolved O 2 gas enables hypoxia relief for enhanced Ce6-mediated PDT. This H 2 O 2 /O 2 self-supplying strategy significantly amplifies the tumor oxidative damage and gains an optimal treatment outcome, which offers a new paradigm for optimizing the tumor therapeutic options limited by oxide or hyperoxide deficiency, not only for CDT/PDT, but also other oxy-substrates involved strategies. Statement of significance The shortage of oxy-substrates in the tumor microenvironment remains a great challenge for ROS-based cancer therapy. Herein, we introduce human serum albumin as a scaffold to stabilize copper peroxide nanomaterials for constant production of H 2 O 2 and O 2 to enhance chemodynamic/photodynamic therapy. The tumor pH-triggered H 2 O 2 /O 2 production and Cu 2+ release are confirmed, assuring the strategy of a highly precise, effective way to destroy tumor without any side effects. This work lends new and exciting insights into the engineering design of autocatalytic oxy-substrates self-supply nanoreactor for overcoming the bottlenecks, like the oxy-substrates deficiency of CDT/PDT and the poor stability of metal peroxides, to achieve highly effective chemodynamic/photodynamic therapy.
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高影响因子
ACS Applied Materials & Interfaces
·
2019
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IF 8.456
Zhongxi Xie,Shuang Liang,Xuechao Cai,Binbin Ding,Shanshan Huang,Zhiyao Hou,Ping’an Ma,Ziyong Cheng,Jun Lin
Hypoxia and overexpression of glutathione (GSH) are typical characteristics of the tumor microenvironment, which severely hinders cancer treatments. Here, we design a novel biodegradable therapeutic system, O2–Cu/ZIF-8@Ce6/ZIF-8@F127 (OCZCF), to simultaneously achieve GSH depletion and O2-enhanced combination therapy. Notably, the doped Cu2+ doubles the O2 storage capacity of the ZIF-8 matrix, which makes OCZCF an excellent pH-sensitive O2 reservoir for conquering tumor hypoxia, enhancing the photodynamic therapy (PDT) efficiency of chlorin e6 (Ce6) under 650 nm laser irradiation. Moreover, the released Cu2+ can act as a smart reactive oxygen species protector by consuming intracellular GSH. The byproduct Cu+ will undergo highly efficient Fenton-like reaction to achieve chemodynamic therapy (CDT) in the presence of abundant H2O2. The accompanying O2 will further alleviate hypoxia. The in vitro and in vivo experimental data indicate that OCZCF could cause remarkable tumor inhibition through enhanced synergetic PDT and CDT, which may open up a new path for cancer therapy.
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高影响因子
Science Bulletin
·
2024
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IF 18.8
Zhihong Bi,Anping Zhang,Gongrui Wang,Cong Dong,Pratteek Das,Xiaoyu Shi,Zhong-Shuai Wu
High-voltage and fast-charging LiCoO 2 (LCO) is key to high-energy/power-density Li-ion batteries. However, unstable surface structure and unfavorable electronic/ionic conductivity severely hinder its high-voltage fast-charging cyclability. Here, we construct a Li/Na-B-Mg-Si-O-F-rich mixed ion/electron interface network on the 4.65 V LCO electrode to enhance its rate capability and long-term cycling stability. Specifically, the resulting artificial hybrid conductive network enhances the reversible conversion of Co 3+/4+ /O 2−/ n − redox by the interfacial ion–electron cooperation and suppresses interface side reactions, inducing an ultrathin yet compact cathode electrolyte interphase. Simultaneously, the derived near-surface Na + /Mg 2+ /Si 4+ -pillared local intercalation structure greatly promotes the Li + diffusion around the 4.55 V phase transition and stabilizes the cathode interface. Finally, excellent 3 C (1 C = 274 mA g −1 ) fast charging performance is demonstrated with 73.8% capacity retention over 1000 cycles. Our findings shed new insights to the fundamental mechanism of interfacial ion/electron synergy in stabilizing and enhancing fast-charging cathode materials.
研究领域:
材料科学
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电化学
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能源存储
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2022
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IF 5.518
Wenjing Shen,Dandan Xiang,Junnan Yang,Yanting Tang,Changhui Xin,Quanhui Guo,Xin Yu
In this work, beta zeolite supported Ti 3+ -TiO 2 /CdS heterojunction was prepared for photodegradation of tetracycline under visible-light irradiation, and zeolite served as a support for the high dispersions of the Ti 3+ -TiO 2 nanoparticles . The obtained zeolite/Ti 3+ -TiO 2 /CdS heterojunction showed a relatively high surface areas of approximately 63.2 m 2 g −1 , much higher than those of the prepared Ti 3+ -TiO 2 /CdS (27.1 m 2 g −1 ), Ti 3+ -TiO 2 (36.5 m 2 g −1 ), and CdS (31.1 m 2 g −1 ), strongly demonstrating the significant of zeolite for high dispersion of the Ti 3+ -TiO 2 /CdS composite. Besides, the experimental results also showed that the photocatalytic degradation efficiency could reach 78 % in 3 min for the zeolite/Ti 3+ -TiO 2 /CdS heterojunction, and the corresponding rate constant was as high as 0.788 min −1 , which was 26.90 times that of pristine Ti 3+ -TiO 2 , 2.24 times of pristine CdS , and 2.04 times of the Ti 3+ -TiO 2 /CdS composite, mainly because of the supporting effects of zeolite and the formation of Ti 3+ -TiO 2 /CdS heterostructure for highly enhanced charge separation. In addition, the trapping experiment revealed that the main reactive species involved in tetracycline degradation were attributed to the photo-generated holes and ⸱O 2 - species.
研究领域:
环境科学
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材料科学
·
化学
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
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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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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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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
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材料科学
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储能技术
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纳米材料
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原位表征
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高影响因子
COMPOSITES PART B-ENGINEERING
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2021
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IF 9.078
Yang Zhan,Shao-hua Luo,Jian Feng,Lin Zhang,Xin Liu,Qing Wang,Ya-hui Zhang
The lithium-oxygen batteries (LOBs) have gained extensive interest in the past decade, but are plagued by slow reaction kinetics and induced large-voltage hysteresis. Therefore, developing extremely capable catalysts to enhance catalytic behavior and mitigate oxidation-reduction overpotential of LOBs is of huge challenge and significance. Attributable to their economically friendly and great activity, transition metal oxides (TMO) have incurred lots of attention as alternative electrocatalysts to replace the currently used noble metal-based catalysts. In this work, we fabricate a highly efficient TMO (the MIL-88A heated at 500 °C under protective flow, M8-Fe 3 O 4 @NC-500) electrocatalyst as advanced cathodes, which attributed to its unique structure, numerous dendritic-shaped carbon layer was anchored inplane into the micrometer-long spindle-shaped prisms with evenly distribution and contains abundant Fe–N/Graphitic N active sites. Therefore, the LOBs (based on M8-Fe 3 O 4 @NC-500/AB cathode) deliver superior electrochemical performance with large specific capacities of 14866.1 mAh g −1 , low overpotentials (1.31 V), and steady cycling stability (553 cycles, limited 500 mAh g −1 , under 0.05 mA cm −2 ). Our work provides a novel vision to rationally design and synthesize a powerful TMO electrocatalyst (with the 2D carbon nanosheet coating) for the LOBs cathode.
研究领域:
材料科学
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电化学
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高影响因子
MOLECULAR PHARMACEUTICS
·
2025
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IF 4.5
Xin Yue,Qian Lin,Xiaohang Liu,Zhaoyi Yu,Jiafeng Xu,Xuan Zhu,Jinyan Lin,Aijie Liu
The high intracellular glutathione (GSH) level, naturally hypoxic conditions within the tumor microenvironment, and limited reactive oxygen species (ROS) generation pose significant obstacles to the effectiveness of sonodynamic therapy (SDT). Overcoming these barriers through depletion of GSH and relieving hypoxia offer a promising strategy to enhance SDT effectiveness. Herein, we developed a dendritic tetra-sulfide-bridged mesoporous silica (DTSMO) that encapsulated both chlorin e6 (Ce6) and cerium via channel-limited in situ coordination and is subsequently cloaked with the macrophage cell membrane (MCM) to facilitate efficient reactive oxygen species (ROS)-based therapy via multispecies enzymatic activities. First, this nanosystem exhibited Ce(IV) ions to mimic catalase (CAT)-like activity, converting H2O2 into O2, thereby effectively alleviating tumor hypoxia. Meanwhile, the nanosystem possessed Ce (III)-based peroxidase (POD)-like activity, enabling the conversion of H2O2 into hydroxyl radicals (•OH) while simultaneously depleting GSH. Both in vitro and in vivo experiments demonstrated that GSH depletion exerted a powerful supplementary effect on CDT and SDT, achieving a tumor inhibition rate of up to 96%, without affecting normal tissues during treatment.
研究领域:
纳米医学
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癌症治疗
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活性氧
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酶模拟
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生物材料
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高影响因子
ELECTROCHIMICA ACTA
·
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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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2026
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IF 12.2
Chunyan Zhang,Jiarong Liu,Qing Cao,Tianzeng Chen,Yonghong Wang,Peng Zhang,Hao Li,Biwu Chu,Xiuhui Zhang,Qingxin Ma,Hong He
The coupled chemical transformation of NOx and SO2 plays a pivotal role in the atmospheric sulfur and nitrogen cycles. While these pollutants show negligible gas-phase interrelationship, they exhibit strong synergistic interactions in multiphase aerosol chemistry, yet their underlying reaction mechanisms remain elusive. We demonstrate that O2 serves as the key mediator enabling efficient coupling between aqueous-phase bisulfite (S(IV)) and nitrite (N(III)) through a previously overlooked reaction pathway at environmentally relevant pH (3.0–6.0). Under isolated conditions at pH 4.4, S(IV) undergoes sluggish O2-driven oxidation (4% sulfate yield), whereas N(III) remains oxidation-resistant. In the absence of O2, S(IV)-N(III) redox reactions yield limited sulfate (4%) and N2O, which is consistent with traditional mechanism cognition. Strikingly, the presence of O2 dramatically enhances co-oxidation, simultaneously producing sulfate (43%) and nitrate (36%). Theoretical calculations identify •HSO3 radicals (from HSO3‐/O2 interaction) as key intermediates that combine with O2/NO2‐ to form transient complexes ([•SO5···ONOH]− and [SO3-NO2···•HO2]−), which ultimately decompose into sulfate and nitrate. Observations in Beijing highlight the dominant role of the S(IV)-N(III) synergistic oxidation mechanism in sulfate formation, surpassing the conventional NO2- and O3-driven pathways. This breakthrough enhances our knowledge of atmospheric chemistry, particularly in the coupled cycling of sulfur and nitrogen, including sulfate/nitrate generation and HONO removal dynamics.
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