CHEMOSPHERE
·
2024
·
IF 8.1
Chunyun Gu,Jiabin Li,Wei Zhou,Jiayi An,Liting Tian,Feng Xiong,Wenbo Fei,Yangfan Feng,Jie Ma
1,2,3-Trichloropropane (TCP) is an emerging groundwater pollutant, but there is a lack of reported studies on the abiotic natural attenuation of TCP by iron minerals. Furthermore, perturbation by O 2 is common in the shallow subsurface by both natural and artificial processes. In this study, natural magnetite was selected as the reactive iron mineral to investigate its role in the degradation of TCP under O 2 perturbation. The results indicated that the mineral structural Fe(II) on magnetite reacted with dissolved oxygen to generate O 2 − · and HO·. Both O 2 − · and HO· contributed to TCP degradation, with O 2 − · playing a more important role. After 56 days of reaction, 66.7% of TCP was completely dechlorinated. This study revealed that higher magnetite concentrations, smaller magnetite particle sizes, and lower initial TCP concentrations favored TCP degradation. The presence of <10 mg/L natural organic matter (NOM) did not affect TCP degradation. These findings significantly advance our understanding of the abiotic natural attenuation mechanisms facilitated by iron minerals under O 2 perturbation, providing crucial insights for the study of natural attenuation.
研究领域:
环境科学
·
化学
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DOI
高影响因子
Nature Chemistry
·
2026
·
IF 24.5
Wang Nan,Cui Chunyu,Xu Runjing,Wang Xiaofang,Wu Chaoxin,Pu Qihao,Wang Wentao,Cao Yongjie,Liao Mochou,Wang Fengmei,Wang Yonggang,Chen Yuhui,Ji Xiao,Xia Yongyao,Wang Fei
Magnesium–oxygen (Mg–O 2 ) batteries are considered promising candidates for next-generation energy storage systems due to their high specific energy, low cost and intrinsic safety. However, poor rechargeability remains a critical barrier, largely due to the lack of suitable electrolytes and undesired irreversible cathode reactions. Here we report a rechargeable non-aqueous Mg–O 2 battery enabled by a tailored electrolyte featuring a cage-like Mg 2+ solvation environment. We find that varying ether solvent chain lengths, alongside a tridentate chelating agent, can act coordinately to form a dynamic solvation microreactor. This solvation environment is consistent with the reversible formation of nanocrystalline magnesium peroxide at the cathode and remains compatible with reversible magnesium plating/stripping. The resulting Mg–O 2 batteries achieve a high initial discharge voltage approaching 2.0 V, an ultralow overpotential of 0.35 V, a remarkable round-trip energy efficiency of 80% and over 450 stable cycles. These results highlight a solvation-structure-guided strategy for enabling rechargeable Mg–O 2 batteries and potentially other multivalent metal–air systems.
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DOI
PubMed
高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2025
·
IF 4.7
Qingfang Jiang,Wujian Zhang,Weijian Ge,Yiping Jin,Wenfeng Han,Ying Li,Haodong Tang
Sintering deactivation of loaded precious metal catalysts is a pressing issue in the field, significantly reducing catalyst activity. Among them, the redispersion of carbon-loaded precious metal catalysts under a high-temperature atmosphere suffers from the problem of carbon carriers being prone to carbonization. In this study, the sintered PdZn/AC catalysts could be redispersed at low temperatures by adding the additive Zn. Combined with TEM, XRD, XPS, and other characterization means, it was found that the main reason for the redispersion of the sintered catalysts was that the Zn additive could form an alloy with Pd, which promoted the formation of high-valent Pd species, which exfoliated into small particles by oxidation in the O 2 –CO atmosphere. In addition, the factors that influenced the process (Zn content, redispersion temperature, treatment time, and number of treatments) were investigated using the controlled variable method. The present work presents a new idea for recycling sintered precious metal catalysts.
研究领域:
催化化学
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材料科学
·
化学工程
·
表面化学
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产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Wenjing Yang,Yibing Ji,Chenhang Ding,Xujie Zhang,Wurikaixi Aiyiti,Chongxian He,Cijun Shuai
Reactive oxygen species (ROS) mediated tumor therapeutic strategies have been extensively studied. However, its effectiveness in eliminating tumor cells is inevitably restricted by the hypoxia or the insufficient hydrogen peroxide (H 2 O 2 ) content. To fundamentally address these challenges, an O 2 -independent and stimuli-responsive nanosystem (named CuS@PMS) is ingeniously constructed by loading peroxymonosulfate (PMS: HSO 5 − ) into hollow mesoporous copper sulfide (CuS) to mediate the generation of sulfate radicals (SO 4 − ). The CuS@PMS was then introduced into polycaprolactone (PCL) to prepare into breast meshes by selective laser sintering. Specifically, the released Cu 2+ ions combining with the photothermal property of CuS synergistically activate PMS, ensuring the cascade amplification of SO 4 − . Unlike conventional ROS, the production of SO 4 − independent on the content of O 2 and H 2 O 2 in the tumor microenvironment, characterizing a longer half-life and faster reaction rate, thereby possessing more advantages in antitumor. The results showed that the SO 4 − yield of PCL/CuS@PMS group significantly higher than that of PCL/PMS group, especially under near-infrared (NIR) light. Moreover, the antitumor efficiency of PCL/CuS@PMS + NIR group was 43 % higher than that of PCL/PMS group in an O 2 -independent manner. The study provided a more efficient, highly adaptable and versatile approach for tumor treatment.
研究领域:
生物医学工程
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纳米技术
·
肿瘤治疗
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产品关联
DOI
高影响因子
Journal of Physical Chemistry C
·
2024
·
IF 3.3
Wan Zhong,Yizhuo Fu,Xueqian Chen,Chao Lu
Electrochemiluminescence (ECL) of the luminol-dissolved O2 system has been applied in many fields, but the role of reactive oxygen species (ROS) in potential-resolved ECL of luminol-dissolved O2 remains ambiguous due to the complexity of the ROS production and the difficulty in detecting ROS. In this work, the function of ROS in potential-dependent luminol-O2 ECL was investigated in detail. Interestingly, the four ECL peaks were observed in the potential-resolved ECL profiles, including a cathodic ECL peak at −0.5 V (ECL-1), two anodic ECL peaks at 0.45 V (ECL-2) and 1.3 V (ECL-3), and a broad and flat peak starting from 1.11 V and ending at 0.35 V (ECL-4, a secondary peak) on the reverse scan backward from upper potentials. The impact of ROS on the different ECL channels was investigated. It was found that superoxide radical (O2•–) could promote all of the above four ECL peaks, while hydroxyl radical (HO•) could only facilitate ECL-1, ECL-3, and ECL-4. Additionally, pathways of all ECL peaks were proposed. The investigation on the role of ROS in potential-resolved ECL of luminol-dissolved O2 will guide the rational regulation and potential applications of luminol ECL in various fields.
研究领域:
分析化学
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电化学
·
生物分析
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DOI
高影响因子
Nature Synthesis
·
2025
·
IF 20
Wang Ruizhao,Dai Jie,Zhao Long,Hu Zhiwei,Chen Chien-Te,Kuo Chang-Yang,Zhan Guangming,Shi Yanbiao,Wang Jiaxian,Zou Yunjie,Xu Mingkai,Zou Xingyue,Zheng Qian,Zhou Bing,Wang Kaiyuan,Zhao Rui,Zhang Yan,Shen Yunhao,Yao Yancai,Zhang Lizhi
Electrochemical O 2 activation offers a green approach for efficient synthesis of singlet oxygen ( 1 O 2 ). However, it is commonly determined by adsorption-dependent O 2 activation and transformation and can suffer from the sluggish desorption of surface-bound *OOH. Here we report an adsorption-independent O 2 activation pathway for 1 O 2 electrosynthesis via an O 2 mono-hydrogenation process on compressive-strained rutile TiO 2 (CSR-TiO 2 ). This CSR-TiO 2 achieved an 1 O 2 generation rate of 148.26 μmol l −1 min −1 with near 100% Faradaic efficiency, outperforming the strain-free counterpart (35.97 μmol l −1 min −1 ) and other previously reported materials. Such superior performance of CSR-TiO 2 stemmed from compressive strain, which can suppress the formation of reductive unsaturated sites for the O 2 adsorption and enhance the reductive ability of atomic hydrogen (H*), favouring the O 2 mono-hydrogenation pathway and bypassing the traditional surface-bound *OOH desorption pathway. The generated 1 O 2 could be utilized for the selective oxidation of thioanisole and its derivatives, offering a promising strategy for green organic synthesis.
研究领域:
材料科学
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电化学
·
绿色合成
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DOI
高影响因子
MOLECULES
·
2025
·Vol. 30
·期 5
·1133
·
IF 4.6
Yuansong Zhou,Fengyu Gao,Lei Yi,Junyi Wang,Honghong Yi,Xiaolong Tang
In an O 2 -containing environment, achieving efficient selective catalytic reduction of nitrogen oxides (NOx) by carbon monoxide (CO) using non-noble metal catalysts remains a formidable challenge. To balance the catalytic oxidation of CO and the catalytic reduction of NOx, we need to develop a catalyst with strong reductibility and weak oxidizability for the CO selective catalytic reduction of NOx (CO-SCR) reaction in the presence of O 2 . In this study, we synthesized the CoCeOx-PVP catalyst via a coprecipitation method and employed various characterization techniques, including BET, SEM, XRD, Raman, XPS, H 2 -TPR, and O 2 -TPD. The analysis results indicate that the addition of polyvinylpyrrolidone (PVP) alters the surface structure of the catalyst, increases the particle size, and enhances the concentration of surface oxygen vacancies. These structural effects facilitate electron circulation and accelerate the migration of oxygen species, thereby improving the catalytic reduction performance of the catalyst and increasing the conversion rate of NOx. At 250 °C and with 5 vol% O 2 , the conversion rates of NOx and CO can attain 98% and 96%, respectively, accompanied by a remarkable N 2 selectivity of 99%. Following a sustained reaction period of 6 h, the conversion efficiencies of both NOx and CO remain above 95%. However, during extended testing periods, as the oxygen vacancies are progressively occupied by O 2 , the oxygen vacancies generated through the reduction of NO with CO fall short of sustaining the CO-SCR reaction over the long haul. Subsequently, the oxidation reactions of NO and CO come to dominate, resulting in a decline in the NOx conversion rate. Notably, the CO conversion rate still maintains 100% at this point. Based on the results of in situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) experiments, we proposed a reaction mechanism for the CO-SCR process over the CoCeOx-PVP catalyst under O 2 -containing conditions. This study provides an effective strategy for the application of non-noble metal catalysts in the field of CO-SCR. Although maintaining long-term activity of the catalyst remains a challenge in the presence of O 2 , the catalyst in this study exhibits a slower deactivation rate compared to traditional non-noble metal catalysts.
研究领域:
催化化学
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环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Tianchang Miao,Ximeng Lv,Fangshuai Chen,Gengfeng Zheng,Qing Han
Achieving O 2 photoreduction to H 2 O 2 with high selectivity control and durability while using easily accessible catalyst requires new synthesis strategies. Herein, we propose an asymmteric Sb coordination active center strategy of introducing anthraquinone (AQ) and heptazine to form local N 3 − Sb − O coordination by a rapid and simple explosive crystallization approach, resulting in a mesoporous conjugated heptazine-amide-AQ polymer coordinated Sb (HAAQ-Sb). It is demonstrated that the N 3 − Sb − O coordination effectively suppresses the charge recombination and acts as the highly active site for O 2 adsorption. Moreover, as-introduced AQ units initiate low-barrier hydrogen transfer through a reversible redox process that triggers highly-efficient H 2 O 2 production. A superior apparent quantum yield of 20.2 % at 400 nm and a remarkable solar-to-chemical conversion efficiency of 0.71 % are achieved on the optimal HAAQ-Sb, which is the highest among C 3 N 4 -based photocatalysts at present. This asymmetric coordination concept and material design method provide new perspectives for the research of novel catalysts toward artificial photosynthesis.
研究领域:
材料科学
·
光催化
·
化学工程
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产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Qiang Zhou,Yi Wan,Xinyu Wang,Qinhua Zhang,Haonan Zhang,Chong Qi,Ziyu Liu,Hao Yang,Tao Xing,Mingqing Wang,Mingbo Wu,Wenting Wu
Photocatalytic oxidation of methane to methanol is a promising process under mild conditions, nevertheless confronting great challenges in achieving high yield and selectivity of methanol simultaneously. Herein, we propose a strategy for the proper amount of hydroxyl radicals (•OH) generation from O 2 by rational design of Au nanoparticles and oxygen vacancies (OVs) co-decorated ZnO photocatalysts. For photocatalytic methane oxidation at ambient temperature, a high CH 3 OH yield of 6.3 mmol·g −1 ·h −1 with a nearly 100 % selectivity has been achieved over the optimized Au 2.5 -def-ZnO (2.5 wt% Au and OVs co-decorated ZnO) photocatalyst, exceeding most reported literatures. Mechanism investigations revealed that Au nanoparticles and OVs synergistically promoted charge separation, improved the adsorption and activation of CH 4 and O 2 , facilitating the selective generation of •OH from O 2 . Combined with the aqueous phase system, the over-oxidation of CH 3 OH was effectively inhibited, thereby achieving high yield and high selectivity of CH 3 OH simultaneously. This work provides some guidance for the design of high-performance photocatalysts for photocatalytic selective oxidation of methane to methanol.
研究领域:
化学工程
·
材料科学
·
环境科学
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DOI
高影响因子
Journal of the American Chemical Society
·
2024
·
IF 14.4
Yao Song,Xiao Yang,Huan Liu,Suxia Liang,Yafeng Cai,Wenqiang Yang,Kaixin Zhu,Liang Yu,Xiaoju Cui,Dehui Deng
Electrochemical conversion of CH4 to easily transportable and value-added liquid fuels is highly attractive for energy-efficient CH4 utilization, but it is challenging due to the low reactivity and solubility of CH4 in the electrolyte. Herein, we report a high-pressure electro-Fenton (HPEF) strategy to establish a hetero-homogeneous process for the electrocatalytic conversion of CH4 by O2 at room temperature. In combination with elevation of reactant pressure to accelerate reaction kinetics, it delivers an unprecedented HCOOH productivity of 11.5 mmol h–1 gFe–1 with 220 times enhancement compared to that under ambient pressure. Remarkably, an HCOOH Faradic efficiency of 81.4% can be achieved with an ultralow cathodic overpotential of 0.38 V. The elevated pressure not only promotes the electrocatalytic reduction of O2 to H2O2 but also increases the reaction collision probability between CH4 and •OH, which is in situ generated from the Fe2+-facilitated decomposition of H2O2.
研究领域:
环境科学
·
电化学工程
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产品关联
DOI
PubMed
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2019
·Vol. 25
·期 12
·3112-3118
·
IF 5.16
Zhipeng Lin,Hao Zhang,Guofeng Liang,Yanqi Jin,Hongbin Zeng,Jiawang Li,Jian Chen,Weihong Zhang,Fangyan Xie,Yanshuo Jin,Hui Meng
Graphical Composite nanostructured cathode : FeOOH nanocubes with a core–shell structure and anchored on carbon ribbons have been prepared. The carbon ribbons improve the conductivity of the system and make more of the FeOOH surface available for electrochemical reaction. An Li/O 2 battery with FeOOH as the cathode material shows a specific capacity of 14816 mAh g −1 cathode and a long-term stability of 67 cycles over 400 h (see figure). A composite of FeOOH nanocubes anchored on carbon ribbons has been synthesized and used as a cathode material for Li/O 2 batteries. Fe 2+ ion-exchanged resin serves as a precursor for both FeOOH nanocubes and carbon ribbons, which are formed simultaneously. The as-prepared FeOOH cubes are proposed to have a core–shell structure, with FeOOH as the shell and Prussian blue as the core, based on information from XPS, TEM, and EDS mapping. As a cathode material for Li/O 2 batteries, FeOOH delivers a specific capacity of 14816 mA h g −1 cathode with a cycling stability of 67 cycles over 400 h. The high performance is related to the low overpotential of the oxygen reduction/evolution reaction on FeOOH. The cube structure, the supporting carbon ribbons, and the -OOH moieties all contribute to the low overpotential. The discharge product Li 2 O 2 can be efficiently decomposed in the FeOOH cathode after a charging process, leading to higher cycling stability. Its high activity and stability make FeOOH a good candidate for use in non-aqueous Li/O 2 batteries.
研究领域:
材料科学
·
能源存储与转换
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DOI
PubMed
高影响因子
Acta Pharmaceutica Sinica B
·
2021
·
IF 11.614
Xiaojuan Zhang,Chuanchuan He,Yun Sun,Xiaoguang Liu,Yan Chen,Chen Chen,Ruicong Yan,Ting Fan,Tan Yang,Yao Lu,Jun Luo,Xiang Ma,Guangya Xiang
Drug transportation is impeded by various barriers in the hypoxic solid tumor, resulting in compromised anticancer efficacy. Herein, a solid lipid monostearin (MS)-coated CaO 2 /MnO 2 nanocarrier was designed to optimize doxorubicin (DOX) transportation comprehensively for chemotherapy enhancement. The MS shell of nanoparticles could be destroyed selectively by highly-expressed lipase within cancer cells, exposing water-sensitive cores to release DOX and produce O 2 . After the cancer cell death, the core-exposed nanoparticles could be further liberated and continue to react with water in the tumor extracellular matrix (ECM) and thoroughly release O 2 and DOX, which exhibited cytotoxicity to neighboring cells. Small DOX molecules could readily diffuse through ECM, in which the collagen deposition was decreased by O 2 -mediated hypoxia-inducible factor-1 inhibition, leading to synergistically improved drug penetration. Concurrently, DOX-efflux-associated P-glycoprotein was also inhibited by O 2 , prolonging drug retention in cancer cells. Overall, the DOX transporting processes from nanoparticles to deep tumor cells including drug release, penetration, and retention were optimized comprehensively, which significantly boosted antitumor benefits.
研究领域:
药学
·
纳米技术
·
癌症研究
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化疗
·
药物递送系统
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产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）