DESALINATION
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2024
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IF 8.3
Xu Yin,Renping Li,Wei Li,Zhifeng Gao,Kajia Wei,Hongwei Zhu,Liankai Gu,Yun Jiang,Weiqing Han
Br − -containing wastewater has the risk of increasing Br − levels in receiving bodies if released into aquatic environments. Electrochemical oxidation is regarded as an ideal method for Br − removal and Br 2 extraction because of its simple procedure and high efficiency. In this work, a novel oxygen vacancy enriched Ti/O v -Co 3 O 4 -NRs electrode was fabricated and used for Br − removal and Br 2 extraction in Br − -containing wastewater. Characterization and experimental results showed that the Ti/O v -Co 3 O 4 -NRs electrode has more prominent bromine evolution reaction (BER) performance than several commercial electrodes (graphite, Ti/RuO 2 -Ir, Ti/PbO 2, etc.). Notably, the construction of oxygen vacancies obviously accelerated the removal of Br − (53 % improvement) by facilitating Br − adsorption and electron transfer. In addition, the influence factors such as initial pH, initial Br − concentration, current density, coexisting ions and temperature on Br − removal were optimized. The Ti/O v -Co 3 O 4 -NRs electrode also exhibited highly stable catalytic activity and conductivity. After 10 cycles, the removal rate of Br − decreased by 2.20 %, and the yield of Br 2 decreased by 3.6 %. In actual applications, the unit energy consumption reached 1.59–1.76 kJ·g −1 Br, and the current efficiency remained above 70 % throughout the whole treatment process. In addition, >80 % of the TOC could be removed during Br 2 extraction, which was more acceptable than the current reported experimental value of electrochemical Br 2 extraction and exhibited great application prospects.
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Muhua Chen,Yuqing Wang,Mengting Li,Bo Fu,Jihuai Tan,Licheng Li,Meisi Chen
The construction of efficient interfacial active sites in metal oxides remains a major challenge for driving the CO 2 cycloaddition under mild conditions. Herein, we engineered a Co x Mg 1-x O solid solution catalyst via a controlled reduction strategy, which achieves near-atomic dispersion within the MgO lattice. The catalyst delivers 96 % yield of cyclic carbonate from epichlorohydrin at 90 °C and 0.1 MPa CO 2 , surpassing the performance of benchmark MgO and Co 3 O 4 catalysts and maintaining stability over five cycles. Structural and spectroscopic characterization (XRD, XPS, UV-Vis) combined with DFT calculations reveal that the high activity originates from synergistic Co-O V -Mg interfacial sites, where Lewis acidic Co 2 + activates epoxides and adjacent oxygen vacancies facilitate CO 2 adsorption. This synergistic effect lowers the energy barrier for the rate-determining ring-opening step to 0.37 eV. This work demonstrates the rational design of oxide solid solutions to create cooperative interfacial sites for efficient CO 2 conversion under mild conditions.
研究领域:
催化化学
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材料科学
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二氧化碳利用
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多相催化
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可持续化学
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yao Zhang,Ruixue Bai,Fanyong Yan,Yidi Wang,Yu Wang,Juanru Huang
Metal-organic frameworks (MOFs) have attracted wide attention owing to unique structural advantages and excellent catalytic properties, yet the inherent poor conductivity and limited visible-light responsiveness constrain their practical applications. Herein, a dual modification strategy based on the thermal decomposition of ligands to construct nitrogen-doped carbon dots (NCDs) decorated MIL-53(Fe) with oxygen vacancies (Ov) is reported in this work. By selectively removing thermally unstable ligands from the dual-ligand MIL-53(Fe) at elevated temperatures, oxygen vacancies were successfully introduced into the MOF framework while maintaining structural integrity. The subsequently integrated amino-rich NCDs facilitated interfacial charge transfer and contributed to improved light utilization. The optimized NCDs@Ov-MIL-53 composites exhibited excellent photocatalytic performance for the degradation of tetracycline. Under visible light irradiation, a removal rate of 93.72 % was achieved within 60 min, which was 2.8 times higher than that of the original MIL-53 (Fe). Systematic characterization showed that oxygen vacancies promoted carrier separation and created active sites, while NCDs acted as electron acceptors. A new insight into defect engineering through ligand-selective pyrolysis is provided by this work and offers a viable strategy for the design of MOF-based photocatalysts for environmental applications.
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DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-14
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IF 14.7
Ye Runping,Ma Lixuan,Mao Jianing,Wang Xinyao,Hong Xiaoling,Gallo Alessandro,Ma Yanfu,Luo Wenhao,Wang Baojun,Zhang Riguang,Duyar Melis Seher,Jiang Zheng,Liu Jian
CO 2 hydrogenation to chemicals and fuels is a significant approach for achieving carbon neutrality. It is essential to rationally design the chemical structure and catalytic active sites towards the development of efficient catalysts. Here we show a Ce-CuZn catalyst with enriched Cu/Zn-O V -Ce active sites fabricated through the atomic-level substitution of Cu and Zn into Ce-MOF precursor. The Ce-CuZn catalyst exhibits a high methanol selectivity of 71.1% and a space-time yield of methanol up to 400.3 g·kg cat −1 ·h −1 with excellent stability for 170 h at 260 °C, comparable to that of the state-of-the-art CuZnAl catalysts. Controlled experiments and DFT calculations confirm that the incorporation of Cu and Zn into CeO 2 with abundant oxygen vacancies can facilitate H 2 dissociation energetically and thus improve CO 2 hydrogenation over the Ce-CuZn catalyst via formate intermediates. This work offers an atomic-level design strategy for constructing efficient multi-metal catalysts for methanol synthesis through precise control of active sites.
研究领域:
催化
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化学工程
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材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
Green Energy & Environment
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2021
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IF 8.207
Weiyao Yang,Mengchen Fu,Chenyu Yang,Yiwen Zhang,Chun Shen
Despite wide applications of noble metal-based catalysts in 5-hydroxymethylfurfural (HMF) oxidation, promoting the catalytic performance at low loading amounts still remains a significant challenge. Herein, a series of metal oxide modified MO x -Au/TiO 2 (M = Fe, Co, Ni) catalysts with low Au loading amount of 0.5 wt% were synthesized. Addition of transition metal oxides promotes electron transfer and generation of the Au δ − –O v –Ti 3+ interface. A combination study reveals that the dual-active site (Au δ − -O v -Ti 3+ ) governs the catalytic performance of the rate-determining step, namely hydroxyl group oxidation. Au δ − site facilitates chemisorption and activation of O 2 molecules. At the same time, O v -Ti 3+ site acts as the role of “killing two birds with one stone”: enhancing adsorption of both reactants, accelerating the activation and dissociation of H 2 O, and facilitating activation of the adsorbed O 2 . Besides, superoxide radicals instead of base is the active oxygen species during the rate-determining step. On this basis, a FDCA yield of 71.2% was achieved under base-free conditions, complying with the “green chemistry” principle. This work provides a new strategy for the transition metal oxides modification of Au-based catalysts, which would be constructive for the rational design of other heterogeneous catalysts.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
Nanoscale Horizons
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2024
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IF 8
Yingnan Qin,Tongzhu Han,Ligang Chen,Kexin Yan,Jing Wang,Ning Wang,Baorong Hou
Marine biofouling severely limits the development of the marine economy, and reactive oxygen species (ROS) produced by electrocatalytic antifouling techniques could inactivate marine microorganisms and inhibit the formation of marine biofouling. Compared with an electro-Fenton reaction, a three-electron oxygen reduction reaction (3e− ORR) could generate a hydroxyl radical (˙OH) in situ without the limitation of pH and iron mud pollutants. Herein, Ov-rich γ-MnO2 is designed to enhance the 3e− ORR performance in neutral media and exhibits excellent sterilization performance for typical marine bacteria. DFT calculation reveals that Ov is beneficial to the “end-on” adsorption and activation of O2, and the Mn site could accept the electrons from *OOH and promote its further reduction to form ˙OH; Ov and Mn sites together guarantee the high 3e− ORR efficiency. In addition, liquid chromatography–tandem mass spectrometry (LC–MS/MS) proves the vast formation of ˙OH in the primary reaction stage, which is the key to sterilization. This work explores the reaction mechanism of the 3e− ORR in neutral media and provides the possibility for the application of electrocatalysis technology in the treatment of marine biofouling pollution.
研究领域:
电化学
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材料科学
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环境科学
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海洋生物学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Junying Tian,Qingxia Guo,Tao Wei,Yongle Guo
The electrochemical CO 2 reduction reaction (ECO 2 RR) offers a route to convert CO 2 into value-added chemicals such as ethylene (C 2 H 4 ). However, this process is constrained by the low content and poor stability of Cu + species, which severely limits the selectivity for C 2 products. To address this issue, we designed CuCe-based oxide catalysts, tuning both the morphology of CeO 2 supports and the Cu loading to maximize the abundance of interfacial Cu + -O V -Ce 3+ motifs and thereby enhance both the content and stability of Cu + species. The resulting optimized catalyst, 10CuCe-S (CeO 2 nanospheres with 10 wt% Cu loading), achieves a C 2 H 4 Faradaic efficiency of 40.2% and a partial current density of 6.63 mA cm −2 at −1.2 V vs. RHE. Structural analyses confirm that the optimal support nanosphere structure and 10 wt% Cu loading give the richest Cu + -O V -Ce 3+ interfacial configuration, leading to a high Cu + density of 69.2% in the 10CuCe-S catalyst, which also exhibits excellent Cu + stability. In situ attenuated total reflection surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) reveals key intermediates (*COOH, *CO, *CHO, *COH) along with rich *COCO species on 10CuCe-S, indicating that abundant Cu + sites facilitate C-C coupling toward C 2 H 4 formation.
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产品关联
DOI
高影响因子
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2026
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IF 5.4
Yang Gao,Xian Du,Zhuo Li,Lihan Wang,Bo Tian,Ruixue Tian,Huiling Du
With the development of industry, large quantities of volatile organic compounds (VOCs) not only cause damage to the ecological environment, but also pose a serious threat to human health. At present, most photocatalysts used for benzene treatment still suffer from problems such as narrow light absorption range, high electron-hole recombination rate, and low charge transfer efficiency. Therefore, the development of high-performance photocatalysts is extremely urgent. The introduction of oxygen vacancies and the construction of heterojunctions can effectively solve the above problems. In this study, a defect-rich photocatalyst was combined with a topology-structured metal-organic framework (MOF) to construct a tightly coupled heterojunction, aiming to address these issues and improve the photocatalytic degradation performance of benzene. By introducing oxygen vacancy-rich TiO₂ nanosheets into NH₂-MIL-125, a tightly coupled Z-scheme heterojunction composite photocatalyst is fabricated. The benzene degradation efficiency of the composite reaches up to 98.5%, which is 1.47 times and 1.27 times that of pure NH₂-MIL-125 and oxygen vacancy-rich TiO₂, respectively, while also exhibiting remarkable stability and high adsorption capacity. Oxygen vacancies act as active sites that strengthen the interfacial electronic interaction of the composite, thereby optimizing the electron transport pathway of the heterojunction and improving the carrier separation efficiency. Under the dual modulation of the heterojunction and oxygen vacancies, the built-in electric field is further intensified, leading to a significant enhancement in the adsorption and catalytic performance of the composite. This study provides an effective design strategy for utilizing oxygen vacancy-driven heterojunctions in catalysts for the efficient abatement of VOCs.
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yunlei Zhang,Yu Cao,Changhao Yan,Wenyun Liu,Yao Chen,Wen Guan,Fang Wang,Yiran Liu,Pengwei Huo
Upgrading bioderived 5-hydroxymethylfurfural (HMF) to high value-added bioplastic monomer 2,5-furandicarboxylic acid (FDCA) is a promising route for biomass conversion. Developing an efficient supported metal catalyst and clarifying the structure–activity relationship between the support and active sites is the key to boost FDCA production. Herein, ZrO 2 coated on natural and abundant halloysite nanotubes (HNTs) was synthesized and employed as a support for Au nanoparticles loading. The Au-ZrO x interface active sites were successfully engineered, and the active site amount can be rationally tailored by adjusting the crystal phases of ZrO 2 via changing calcination temperature. A combination study of catalysts surface physicochemical properties and catalytic activity reveals that oxygen vacancies (O v ) play a vital role in enhancing the adsorption of O 2 . Meanwhile, interface active sites facilitate the chemisorption and activation of O 2 molecules, which makes it easier to produce oxygen active species (superoxide radicals). More importantly, in-situ infrared spectroscopy and adsorption experiments also demonstrate that the catalyst with a higher O v concentration not only contributes to a stronger Lewis acid intensity, but also enhances the adsorption capacity of a key intermediate 5-hydroxymethyl-2-furancarboxylic acid (HMFCA), thus leading to an acceleration of the rate-determining step of hydroxyl group oxidation. The highest 99.4 % of FDCA yield can be obtained in 3.0 h. This newly proposed model of interface active sites may shed a light on the design of novel heterogeneous catalysts for the related biomass oxidation reactions.
研究领域:
催化
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材料科学
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化学工程
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生物质转化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yujiao Zhang,Yan Wang,Zhao Hu,Jinshu Huang,Song Yang,Hu Li
Exploring the real force that drives the separation of Coulomb-bound electron-hole pairs in the interface of heterojunction photocatalysts can establish a clear mechanism for efficient solar energy conversion efficiency. Herein, the formation of oxygen vacancy (Ov) and isolated Ti 3+ was precisely regulated at the interface of g-C 3 N 4 /TiO 2 Z-scheme heterojunction (g-C 3 N 4 /Ov-Ti 3+ -TiO 2 ) by optimizing the opening degree of the calcination system, showing excellent production rate of CO and CH 4 from CO 2 photoreduction under visible light. This photocatalytic system also exhibited prominent stability. Combining theoretical calculation and characterization, the introduction of Ov and isolated Ti 3+ on the interface could construct a charge transfer channel to break the forbidden transition of n → π*, improving the separation process of photoexcited electron-hole pairs. The photoexcited electrons weakened the covalent interaction of C O bonds to promote the activation of adsorbed inert CO 2 molecules, significantly reducing the energy barrier of the rate-limiting step during CO 2 reduction. This work demonstrates the great application potential of reasonably regulating heterojunction interface for efficient photocatalytic CO 2 reduction.
研究领域:
材料科学
·
环境科学
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产品关联
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2026
·
IF 2.6
Zehua Yuan,Munire Tuerhong,Jinhua Liang,Xirenayi Aisikaer,Jubao Zhang,Gulgina Mamtmin
Photocatalytic technology based on a heterojunction structure has been demonstrated as an effective approach to address environmental pollution and energy issues. In this study, an oxygen-vacancy (Ov)-rich S-scheme BiVO4/Bi-TCPP heterojunction was fabricated via a facile hydrothermal method for the degradation of tetracycline (TC) and oxytetracycline (OTC), and innovatively applied to wheat seed germination experiments to evaluate the ecological safety of treated water samples. A series of characterization results indicate that the one-step strategy enables the in situ introduction of oxygen vacancies and simultaneous heterojunction construction, avoiding complex post-treatment processes. The oxygen vacancies generate defect sites and electron trapping centers, effectively narrowing the band gap, enhancing visible light absorption capacity, and promoting the separation of photogenerated carriers. The S-scheme heterojunction formed by BiVO4/Bi-TCPP coupling effectively facilitates charge transfer, further promotes carrier separation, and improves photocatalytic activity. Under visible light irradiation, the optimized system achieved a TC degradation rate of 90.15% within 90 min and an OTC degradation rate of 85.30% within 120 min, with excellent stability. In addition, the photocatalytic degradation mechanism and dominant active species of the Ov-rich S-scheme BiVO4/Bi-TCPP heterojunction were investigated. Wheat seed germination experiments confirmed that the phototreated antibiotic wastewater significantly reduced the inhibitory effects on the wheat seed germination rate and root elongation, demonstrating that this system not only efficiently removes antibiotics but also effectively eliminates their ecological toxicity, ensuring the environmental safety of the effluent. This study provides new insights into the Ov-regulated S-scheme photocatalytic degradation of TC and OTC and broadens its potential application in wastewater remediation.
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yu Su,Rong Fan,Jiabao Li,Yangxi Liu,Ziyuan Zheng,Xin Zhou,Xiang Feng,Yibin Liu,Hui Zhao,Xiaobo Chen,Xingong Zhang,Chaohe Yang,Hao Yan
Oxidation of fatty alcohols to fatty acids is still challenging due to the sluggish activation of the C–H bond over Au supported on reducible oxides with a coordination-saturated structure. Herein, we constructed an efficient interfacial Auδ−–OV–Ti structure by tuning the crystal forms of TiO2. Compared with TiO2-rutile exposed by (110) and (111) crystal facets, TiO2-anatase can exploit the defect (101) crystal facet to obtain rich oxygen vacancies (OV), inducing electron migration from TiO2-anatase support to Au species to form electron-rich Auδ− species. Specifically, the synergistic catalytic effect between the OV–Ti and Auδ− species greatly enhances the adsorption of alcohol and thereby overcomes sluggish activation of the C–H bond caused by the electron pushing effect triggered by long carbon chains. Consequently, the Au/TiO2-anatase catalyst shows excellent isooctyl alcohol conversion (69.5%) and isocaprylic acid selectivity (67.9%) under base-free conditions. The catalytic system is further extended to the oxidation of other fatty alcohols to fatty acids with excellent catalytic performance.
研究领域:
催化化学
·
材料科学
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DOI
高影响因子
危险品化学品经营许可证（带存储）