Environmental Science-Nano
·
2023
·Vol. 10
·期 11
·3072-3083
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IF 7.3
Chuanqi Pan,Biluan Zhang,Tingyu Pan,Hui Huang,Siyi Song,Xitong Cai,Yuhang Wang,Hongwei Sun,Zhu Luo,Lizhi Zhang,Yanbing Guo
The dual activation mechanism of molecular oxygen (O2) and water (H2O) in the local structure of catalysts has not been elucidated yet. Herein, we report a strategy for manufacturing fully exposed Ag4 sites in nano silver/graphdiyne (Ag/GDY) composites for activating O2 and H2O. The synthesized nano Ag was uniformly anchored on the surface of GDY without any surfactant added, with an average particle size of 2.5 nm. The unique sp-hybrid C and triangular pore structure of GDY not only regulate the stable geometric structure of nano Ag, but also enhance the adsorption ability of Ag4 sites for O2 and H2O molecules in nano Ag/GDY. Electron spin resonance spectroscopy and density functional theory calculation results proved that O2 is more favorable to synergistically promote the activation of H2O to generate reactive ·O2− and ·OH radicals on the nano Ag/GDY surfaces, leading to outstanding antibacterial activity. This work provides a simple strategy for the preparation of stable nano Ag and proposes to improve the catalytic oxidation activity by adjusting the local electronic structure of catalysts to activate O2 and H2O.
研究领域:
材料科学
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催化化学
·
微生物学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANIC CHEMISTRY
·
2019
·
IF 4.745
Na Li,Jinku Bai,Xiaolin Zheng,Honghua Rao
An iron-catalyzed methylene forming strategy is disclosed through sequential C–H and C–O bond functionalization of methanol with cosolvent water. This protocol provides an easy and novel access to methylene-tethered imidazo[1,2-a]pyridine and 2-aminopyridine analogues in a sustainable manner and represents a complementary approach to traditional methylene forming strategies.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 39
·18744-18750
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IF 3.925
Dawang Chu,Hui Zhou,Zhicheng Luo
Selective conversion of glycerol to lactic acid requires the synergistic activation of C–H, C–O, and O–H. Herein, we report an inexpensive Fe–Cr/TiO2 catalyst that achieves lactic acid formation with a high selectivity of 60.5%. By changing the Fe/Cr ratios and reduction temperatures, the structures of Vő and Vő-OH were altered, which determined the overall oxidation–dehydration–isomerization process. The in situ ATR-IR experiments confirmed the activation of glycerol by adsorbing the primary −OH, and a series of control experiments verified that Fe was responsible for the cleavage of C–H and O–H, while CrOx catalyzed the activation of C–O and C–H. This work designs a hydrothermal catalyst with multifunctional ability, which may guide the rational catalyst design for the selective oxidation of glycerol to lactic acid.
研究领域:
催化化学
·
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2020
·
IF 7.888
Jian Zhang,Yazhe Zhang,Jieqiong Zhao,Zhe An,Yanru Zhu,Xin Shu,Hongyan Song,Xu Xiang,Xiaodan Ma,Jing He
Oxidative carbonylation has attracted broad interest from both academia and industry in recent years. Oxycarbonylation of ethanol to diethyl carbonate (DEC) has been of great challenge due to the difficulty in the simultaneous activation of ethanol and CO. This work reports a heterogeneous Cu-Pd pair catalysis for simultaneous activation of ethanol and CO, affording a selectivity of 85.4% to DEC and a space–time yield (STY) of up to 207 mg∙g −1 ∙h −1 . Well distributed Cu-Pd pair affords more Cu (I) sites, promoting CO activation and the followed insertion to adsorbed ethanol. Further increasing ratio of Cu (I) species via the pre-treatment of catalyst with CO and ethanol promotes simultaneously the activation of ethanol and CO, affording a STY of 325 mg∙g −1 ∙h −1 of DEC.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yaping Zhang,Yanan Zhao,Yixin Qi,Yanyan Lin,Yuhang Cheng,Mengmeng Sun,Lei Wang
Photogenerated holes have emerged as critical mediators for activating peroxymonosulfate (PMS) in the coupled photocatalytic PMS activation system, enabling novel dual-channel activation pathway. A tandem system based on Fe-MOF@BiVO 4 (Vis/PMS/Fe-MOF@BVO) with spatially separated active sites was constructed to form a dual-channel activation mechanism. The BiVO 4 (010) face provides the active sites for photogenerated electrons to drive the Fe 3+ /Fe 2+ cycle and activate PMS, while the BiVO 4 (110) face serves as the active sites for photogenerated holes to activate PMS. Consequently, the Vis/PMS/Fe-MOF@BVO system achieved complete degradation of 10 mg/L BPA within 6 min, with a degradation rate constant (K obs ) of 0.74 min −1 . It also demonstrated high removal efficiency for various organic pollutants with excellent immunity to interference and reusability. This work provides a new insight into the coordinative mechanism for coupled photocatalysis and PMS activation system.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Qihao Gui,Libo Zhang,Shixing Wang,Jianjun Fang,Zixing Song,Zhicong Wei,Dianwen Liu
Pyrite enclosure poses a significant challenge in refractory gold ore processing, inhibiting gold leaching. This study explores Sulfate Radical-based Advanced Oxidation Processes (SR-AOPs) as an effective alternative for pretreating such ores. The oxidation pretreatments were performed under heat and ultrasound activation methods, including heat and ultrasound, and the influences of pretreatment time, pH, ultrasound power, pretreatment temperature, and precursor (PDS) concentration were investigated. Both ultrasonic and heat activation effectively mitigate the negative impact of pyrite enclosure on gold leaching. Specifically, the gold leaching rate improved from 21.9 % to 46.1 % and 74.9 % with heat and ultrasound activation, respectively The and generated by PDS dominate the pyrite oxidation according to EPR and quenching tests. Meanwhile, the SR-AOPs treatment also promotes the interactions between pyrite enclosure and leaching agent, reducing the negative influences of pyrite. Kinetic studies indicated that the oxidation processes are different under heat and ultrasound activation. Heat activation is governed by an interfacial chemical reaction, with an activation energy of 25.57 kJ/mol. In contrast, ultrasound-induced cavitation and microjets remove the oxidation layer, disrupt the pyrite crystal structure, and expose encapsulated gold. These effects accelerate pyrite oxidation, shifting the kinetic control step from interfacial chemical reaction to internal diffusion, with a reduced activation energy of 35.06 kJ/mol.
研究领域:
矿物加工工程
·
环境化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Hui Wang,Wangsheng Yu,Xu Peng,Zewen Chen,Shengji Wu,Qinqin Yu,Wei Yang,Jie Zhou
In the present work, highly efficient catalytic adsorbents for Hg 0 removal in both oxygen-rich and deficient atmosphere are developed based on an “adaption” strategy. Firstly, a series of simplified SiO 2 -based catalytic adsorbents are prepared as model catalysts to gain a deeper insight into the mechanism of the catalytic Hg 0 removal process. It is found that for the effective Hg 0 removal, the catalytic adsorbent should possess an “assembling” structure involving both Hg 0 and oxygen activation sites. An “adaption” strategy is thus implemented for the devise of the catalytic adsorbent, including the functional adaption of different active sites for the reactants and the synergistic function of different active sites. Accordingly, high-efficiency catalytic adsorbent with strong redox property is developed for oxygen-rich atmosphere, while the catalytic adsorbent with high oxygen storage/release property is developed for oxygen-deficient conditions. Moreover, regeneration investigation indicates that the activities of spent catalytic adsorbents are almost fully recovered through the temperature programmed decomposition and desorption (TPDD) process. It is believed that the present “adaption” strategy for catalyst design has guiding significance for the rational and controllable construction of catalysts for other catalytic processes.
研究领域:
环境催化
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大气污染控制
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材料化学
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表面科学
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化学工程
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环境功能材料
✓ 已验证
DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2023
·Vol. 30
·期 32
·78279-78293
·
IF 5.8
Arif Muhammad,Liu Guijian,Zia ur Rehman Muhammad,Mian Md Manik,Ashraf Aniqa,Yousaf Balal,Rashid Muhammad Saqib,Ahmed Rafay,Imran Muhammad,Munir Mehr Ahmed Mujtaba
An inexpensive and environmentally friendly composite synthesized from rice husk, impregnated with montmorillonite and activated by carbon dioxide, was investigated for the removal of azithromycin from an aqueous solution. Various techniques were used to characterize adsorbents in detail. The sorption process was primarily regulated by the solution pH, pollutant concentration, contact duration, adsorbent dose, and solution temperature. The equilibrium data were best analyzed using the nonlinear Langmuir and Sips (R 2 > 0.97) isotherms, which revealed that adsorption occurs in a homogenous manner. The adsorption capacity of pristine biochar and carbon dioxide activated biochar-montmorillonite composite was 33.4 mg g −1 and 44.73 mg g −1 , respectively. Kinetic studies identified that the experimental data obeyed the pseudo-second-order and Elovich models (R 2 > 0.98) indicating the chemisorption nature of adsorbents. The thermodynamic parameters determined the endothermic and spontaneous nature of the reaction. The ion exchange, π-π electron-donor–acceptor (EDA) interactions, hydrogen-bonding, and electrostatic interactions were the plausible mechanisms responsible for the adsorption process. This study revealed that a carbon dioxide activated biochar-montmorillonite composite may be used as an effective, sustainable, and economical adsorbent for the removal of azithromycin from polluted water.
研究领域:
环境科学
·
化学工程
·
材料科学
·
水处理
·
吸附技术
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Yanan Huang,Yan Zhao,Dawei Song,Yaqin Shi,Huan Chen,Bo Niu,Donghui Long,Yayun Zhang
This study uncovers a synergistic Fe-Mo dual-atom catalytic mechanism that enhances peroxymonosulfate (PMS) activation and pollutant degradation through dynamic electron management and substrate pre-activation. A nitrogen-doped carbon-supported FeMo dual-atom catalyst (FeMo/NC) was synthesized and systematically analyzed using XAFS, in situ Raman, DFT calculations, and electrochemical tests. The FeMo/NC-PMS system achieved 99 % ciprofloxacin (CIP) degradation within 10 minutes (rate constant: 0.402 min −1 ), maintained > 90 % efficiency across pH 1–13, and exhibited minimal Fe/Mo leaching (<0.1 ppm) with 90 % retention after five cycles. Mechanistic studies revealed that Mo stabilizes Fe valence states via electron transfer, strengthens Fe-N coordination, and promotes pollutant pre-activation on Mo sites while enabling selective 1 O 2 generation at Fe sites. This work establishes a dual-atom design strategy to optimize electron redistribution and interfacial interactions in Fenton-like systems. The demonstrated compatibility with membrane filtration (100 % CIP removal in wastewater) highlights its potential for practical water remediation applications.
研究领域:
环境科学
·
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2011
·
IF 2.072
Juan Yang,Keqiang Qiu
Doehlert matrix was used to optimize the experimental conditions for the preparation of activated carbons from herb residues by vacuum chemical activation and traditional chemical activation using ZnCl2 as activation agent. The effects of activation temperature and impregnation ratio, the most influential factors of ZnCl2 chemical activation, were studied. The obtained activated carbons were characterized by total yield and methylene blue and iodine adsorption value. Each response has been described by a second-order model, and the predicted model presented a good agreement with experimental data. The results showed that activated carbons prepared by vacuum chemical activation have higher yield and better adsorption capacity. The removal percentages of methylene blue for the two optimal activated carbons and a commercial activated carbon were determined. The activated carbon prepared by vacuum chemical activation exhibited the highest methylene blue removal efficiency.
研究领域:
环境科学
·
材料科学
·
化学工程
·
资源循环利用
·
吸附技术
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Miao,Ying Liu,Dandan Wang,Ningjie Du,Ziwei Ye,Yang Hou,Shun Mao,Kostya (Ken) Ostrikov
Transition-metal and nitrogen co-doped carbon-based catalysts receive much attention in peroxymonosulfate (PMS) activation. However, the contribution of doped metal and the kinetic mechanisms of the emerging nonradical pathways especially enabled by reactive singlet oxygen species remain unclear. Herein, we report Fe-N-co-doped carbon-based catalysts (FeCNx) for peroxymonosulfate activation. The catalysts achieve fast removal of a broad spectrum of organic pollutants in a wide pH range without the common Fe leaching. Both catalyst surface-activated PMS complex (catalyst-PMS*), surface-bound radicals, and singlet oxygen are identified. The new mechanism is enabled by the Fe-Nx single-atomic-site that enhances the adsorption of PMS and facilitates the formation of catalyst-PMS*. The formation route of singlet oxygen species is elucidated for the first time for Fe, N-co-doped carbon-based catalysts with density functional theory simulation. This study reveals the intrinsic role of Fe-Nx site in catalysts and provides new insights into the origin and kinetics of non-radical pathways for peroxymonosulfate activation.
研究领域:
环境科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY
·
2024
·
IF 9
Tao Tan,Yushu Chen,Yongyue Wang,Zuhao Li,Zhige Zhang,Jun Xie,Yong Chen
The use of green biogas as a raw material for producing methanol-friendly syngas (H 2 /CO ≈ 2) for one-step methanol synthesis has gained significant attention. However, developing efficient catalysts with high activity and stability remains challenging, as they often face issues with stability and carbon deposition. This study presents a Ni/CeO 2 /HT catalyst designed for high activity and long-term stability by leveraging the Ce redox cycle and strong interactions between Ni-CeO 2 and hydrotalcite (HT). The catalyst benefits from abundant oxygen vacancies generated by the Ce 3+ - Ce 4+ pathway, enhancing its ability to activate CO 2 and H 2 O and providing excellent coke resistance. Comprehensive analyses of CO 2 /H 2 O adsorption and carbon elimination mechanisms were conducted using techniques such as in situ H 2 -TPR, CO 2 /H 2 O-TPSR, in situ CH 4 -TPSR, CO 2 /H 2 O-TPO, and FTIR. The Ni/CeO 2 /HT catalyst outperformed others in CO 2 /H 2 O adsorption and CH 4 activation capacity, promoting the generation of active oxygen species and effectively removing coke precursors, thereby improving resistance to Ni sintering and carbon deposition. At 750 °C and a weight hourly space velocity (WHSV) of 32,400 mLg Cat −1 h −1 , it achieved CH 4 and CO 2 conversions of 93 % and 66 %, respectively, with long-term stability exceeding 200 h.
研究领域:
催化化学
·
可再生能源
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）