SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Fei Yan,Xiaotong Ding,Yanxin Quan,Xiaolong Yang,Haoyu Sun,Juanjuan Qi,Ping Li,Lidong Wang
Dimethyl sulfoxide (DMSO) is an important solvent in numerous industries. The biodegrading process of DMSO is slow and produces toxic volatile compounds including CH 3 SCH 3 , CH 3 SH, and H 2 S. Hence, it is important to develop chemical methods for treating DMSO-containing wastewater. In the present work, niobium oxyhydroxide and niobium oxide were synthesized and used to activate hydrogen peroxide for the degradation of DMSO to DMSO 2 . The niobium oxyhydroxide catalyst exhibited much better catalytic activity for DMSO oxidation than niobium oxide. EPR spectra and radical scavenging experiments confirmed that O 2 •− and 1 O 2 are the main active species for the oxidation of DMSO. FTIR analysis and DFT calculation confirmed that the surface hydroxyl of niobium oxyhydroxide can be substituted by hydroperoxo group of H 2 O 2 to form Nb−OOH group, which can directly oxidize DMSO or indirectly oxidize DMSO via O 2 •− and 1 O 2 . However, H 2 O 2 cannot form hydroperoxo group on the surface of niobium oxide, which might trigger the lower activity of niobium oxide catalysts than the niobium oxyhydroxide catalyst. The niobium oxyhydroxide catalyst exhibited good reusability and was promising for the treatment of DMSO-containing wastewater.
研究领域:
环境化学
·
催化
·
废水处理
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Nano Materials
·
2021
·
IF 5.097
Yuanjie Xiong,Xiang Liu,Tian Cheng Zhang,Shaojun Yuan
The conversion of As(III) to As(V) in groundwater is an urgent issue, owing to the higher mobility, stronger toxicity, and weaker binding ability of As(III). In this work, the electrocatalytic oxidation of As(III) was efficiently achieved with a facile and environmentally benign method by using hierarchical MnO2-deposited TiO2 nanotube arrays (MnO2/TNAs) as the anode. The electrocatalytic oxidation performance of the as-fabricated MnO2/TNA-coated anode was systematically investigated. The results exhibited that such as-fabricated MnO2/TNAs had a high oxidation efficiency of 90% at a low concentration of As(III) (1 mg L–1). Furthermore, the reaction mechanism was systematically studied by electron spin resonance and free radical capture experiments. The oxidation of As(III) was accomplished via both direct oxidation on the anode surface and indirect oxidation of the reactive oxygen species. The highly efficient TNA-based anode offers a potentially promising advanced material for electrochemical oxidation of trace As(III) in the practical field.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Ning Kang,Zhiqiang Zhao,Xiaoyang Yu,Jin Lin,Shouxiang Lu
The application of ceria-supported catalysts as promising catalysts for air pollutant abatement via heterogeneous catalytic processes is still a challenge. Phosphorus (P) is a potential threat to catalyst deactivation but has not been sufficiently explored. Herein, a systematic study reveals the poisoning behaviors of P on Cu-Mn bimetallic oxides supported by ceria (Cu-Mn/CeO 2 ) as a typical case in CO oxidation and provides new insights into the deactivation mechanism. The P impregnation decreases the surface area of Cu-Mn/CeO 2 and leads to the emergence of a new sheet morphology. The interactions between P and catalyst components (support and active species) result in the generation of dominant P species of PO 4 3− and PO 3 − . The P addition also weakens the oxygen storage capacity of ceria and decreases the proportions of low-valent Cu and Mn, hindering electron transfers among metals. Furthermore, the reducibility and the adsorption and activation of O 2 are limited in P-loaded Cu-Mn/CeO 2 catalysts as found in H 2 -TPR and O 2 -TPD when increasing the P concentration. In situ DRIFTS experiments demonstrate that the inhibition of the formation and transformation of active intermediates, namely carbonyls and carbonates, is responsible for the poisoning behaviors of P in the pathway of CO oxidation over Cu-Mn/CeO 2 catalyst.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Archer Bright,Wuyi Zhang,Kaisong Xiang,Hao Chen,Hui Liu,Jun Wu
CuO-CeO 2 composite catalyst for low temperature CO oxidation was fabricated via an impregnation method. The prepared composite CuO-CeO 2 achieved 50 % and 100 % conversion at approximately ∼ 70℃ and ∼ 110℃ (denoted as T 50 and T 100 ), respectively. The enhanced catalytic activities were attributed to the formation of abundant CuO/CeO 2 heterostructures, which increased the concentration of oxygen vacancies in their lattices. In addition, the pore structure of the CuO-CeO 2 composite has also been optimized during the impregnation synthesis process. Compared with bare CeO 2 , which only possesses micropores, CuO-CeO 2 forms more mesopores on its surface, which assists in reducing the deposition rate of sulfate species on the surface. The SO 2 tolerance of the catalyst and hence its stability towards practical industrial flue gas treatment is significantly promoted. Furthermore, Density Functional Theory (DFT) was also performed to explore the mechanism of CO oxidation on the CuO-CeO 2 . It was found that the oxygen vacancy can be easily formed on the CuO/CeO 2 heterointerfaces; the adsorption energy (ΔG) of CO was therefore decreased to 0.15 eV, much lower than that of bare CeO 2 (0.53 eV). Besides, the center of f electrons of Ce in CeO 2 rises from −0.55 eV to – 1.71 eV by introducing CuO, suggesting that the f electrons in Ce become more active, which is beneficial for CO to adsorb.
研究领域:
催化化学
·
环境化学
·
材料科学
·
表面化学
·
工业催化
✓ 已验证
产品关联
DOI
高影响因子
MOLECULES
·
2024
·Vol. 29
·期 7
·1548
·
IF 4.2
Qian Wang,Tianqi Huang,Shuang Tong,Chao Wang,Hongping Li,Ming Zhang
With the increasingly strict limitations on emission standards of vehicles, deep desulfurization in fuel is indispensable for social development worldwide. In this study, a series of hybrid materials based on SiO2-supported polyoxometalate ionic liquid were successfully prepared via a facile ball milling method and employed as catalysts in the aerobic oxidative desulfurization process. The composition and structure of prepared samples were studied by various techniques, including FT-IR, UV-vis DRS, wide-angle XRD, BET, XPS, and SEM images. The experimental results indicated that the synthesized polyoxometalate ionic liquids were successfully loaded on SiO2with a highly uniform dispersion. The prepared catalyst (C16PMoV/10SiO2) exhibited good desulfurization activity on different sulfur compounds. Moreover, the oxidation product and active species in the ODS process were respectively investigated via GC-MS and ESR analysis, indicating that the catalyst can activate oxygen to superoxide radicals during the reaction to convert DBT to its corresponding sulfone in the fuel.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL PHYSICS LETTERS
·
2024
·
IF 2.8
Wen-Meng Gao,Ling-Yu Dong,Wen-Cui Li,Xu Hu,Lei He,Guang-Ping Hao,An-Hui Lu
We report the selective introduction of oxygen-containing functional groups for two-electron oxygen reduction reaction (2e-ORR) in self-supportive carbon electrode using electrochemical oxidation method. The optimal electrode shows hydrogen peroxide (H 2 O 2 ) selectivity up to 95 %. C O is found active to control 2e-ORR selectivity and mechanism of oxygen species variation is elucidated by in situ infrared reflection absorption spectroscopy. We further improve mass transfer by introducing highly interconnected macropores in electrode, which shows H 2 O 2 yield of 144 mmol cm − 2 h −1 and Faradaic efficiency of nearly 100 %. These may inspire advanced active electrode creation for applications through selective electrochemical doping and structural design.
研究领域:
材料科学
·
电化学
·
催化反应
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2024
·
IF 3.8
Yu-Zhen Xu,Yu-Le Wang,Yu-Dong Shan,Song-Hai Wu,Yong Liu,Xu Han
Selective oxidation of cyclohexene (Cy) to cyclohexene oxide (Cy-ep) by O2 under solvent- and initiator-free conditions is a challenge in chemical processes, which is still constrained by its low selectivity (theoretical selectivity of 50.0%). Given the low epoxide selectivity (<20.0%) of single metal catalysts, we propose a relay catalysis strategy on the oxidation of Cy to Cy-ep with high selectivity by the spherical Mg–Mo bimetallic oxide (MMO). Such a relay catalyst exhibits a desirable Cy conversion of 31.0% and a high selectivity of 49.3% toward Cy-ep. Meanwhile, the high stability and reusability of MMO also indicate its potential to be used for industrial scale-ups. A series of characterizations and DFT calculations reveal that the negatively charged lattice oxygen in [MgII–O–II] adsorbs allylic H of Cy to weaken the bond energy of the allylic C–H bond and form Cy•, and then Cy• rapidly traps O2 to give CyOO•, which subsequently abstracts H from allylic C–H of another Cy to form 2-cyclohexene-1-hydroperoxide (Cy-OOH) and Cy•, achieving the propagation cycle. On the other hand, the Mo(VI) site in MMO catalyzes the produced Cy-OOH peroxo, which then oxidizes Cy to Cy-ep and 2-cyclohexene-1-ol. This work provides insight into the relay catalyst for the epoxidation of olefin with O2 with high selectivity under solvent- and initiator-free conditions.
研究领域:
化学工程
·
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chao Feng,Gaoyan Xiong,Fei Jiang,Qianqian Gao,Chong Chen,Yuan Pan,Zhaoyang Fei,Yanpeng Li,Yukun Lu,Chenguang Liu,Yunqi Liu
Through morphology control and structure construction of manganese catalyst to improve the conversion of VOCs is still a significant challenge in the field of environmental catalysis. Herein, secondary sphere structured δ-type manganese oxide (MnO 2 -SS) was synthesized via a simple room temperature two-step method. Compared with other sphere-type MnO 2 samples, MnO 2 -SS exhibited a higher propane oxidation activity (T 90 = 238 ℃), turnover frequency (14.54 × 10 −7 s −1 at 240 ℃), and stability in H 2 O, NO 2 , and CO atmospheres. Experimental results indicated that MnO 2 -SS exhibited an ultrahigh specific surface area, a high surface concentration of active Mn 4+ species and superior surface oxygen mobility. In-situ DRIFTs revealed that active oxygen species exhibit a key role in formation and dissociation of intermediate carboxylates. Electron paramagnetic resonance, O K-edge results and density functional theory calculation revealed that numerous oxygen vacancies existed on MnO 2 -SS. These vacancies can facilitate adsorption and activation of O 2 to generate active reactive oxygen species, which lead to superior propane and intermediate carboxylates oxidation activity. This work provides new strategy to enhance the surface oxygen activity of manganese oxide.
研究领域:
环境催化
·
材料科学
·
化学工程
✓ 已验证
DOI
高影响因子
Desalination and Water Treatment
·
2024
·
IF 1
Zicai Zhao,Yuanyuan Zhang,Shuangfei Wang,Hongxiang Zhu,Jianhua Xiong
ABSTRACT In this study, zinc oxide (ZnO) supported copper oxide (CuO) catalyst was prepared and characterized. Ofloxacin (OFL) was selected as the target pollutant to study the catalytic activity of CuO/ ZnO. The characterizations of CuO/ZnO were studied using X-ray diffraction, field emission scanning electron microscopy and X-ray photoelectron spectroscopy etc. The catalytic activity of CuO/ZnO on OFL degradation efficiency was systematically examined under different experimental conditions: including different catalyst doses, O 3 flow rates, initial pH values and OFL concentrations. The catalytic activity achieved maximal when Cu:Zn was 1:5. The results showed that the degradation of OFL increased with the increase of CuO/ZnO dosage, O 3 flow rate and pH value, but decreased with the increase of OFL initial concentration. Under selected initial conditions (80 mL/min ozone flow, 20 mg/L OFL solution, and 0.63 g/L catalyst dosage), the O 3 +CuO/ZnO process significantly improved OFL removal efficiency due to the production of hydroxyl radical ( • OH), which was approved by tert-butanol (TBA). It was confirmed that CuO and ZnO showed synergistic effect on the catalytic ozonation of OFL. The degradation efficiency of OFL was only slightly decreased after five repeated times, indicating that CuO/ZnO had well catalytic stability.
研究领域:
环境科学
·
催化化学
✓ 已验证
DOI
高影响因子
Arabian Journal of Chemistry
·
2020
·
IF 4.762
Kechen Song,Shuo Wang,Qiang Sun,Deping Xu
Nano-sheets Al 2 O 3 supported CeO 2 -Fe 2 O 3 binary oxides were prepared by the vacuum impregnation method. The structural and textural properties were characterized by pertinent techniques, and the materials were evaluated as catalysts for the oxidative dehydrogenation of ethylbenzene with carbon dioxide (CO 2 -ODEB). The characterization results show that all samples maintain the hierarchical structure, and CeO 2 -like and Fe 2 O 3 -like solid solutions were formed when changing the Ce-to-Fe molar ratio. The catalytic performances indicate that CeO 2 -Fe 2 O 3 binary oxides were effective for CO 2 -ODEB, and the activity is determined by mobile oxygen, which can facilitate the dehydrogenation process. The DFT studies further identified the reaction pathway and rate-determining step. The inter-transmission of oxygen species and the presence of CO 2 refill the oxygen vacancies and restore the redox cycle of CeO 2 -Fe 2 O 3 binary oxides.
研究领域:
催化化学
·
材料科学
·
理论计算化学
✓ 已验证
产品关联
DOI
高影响因子
COMPOSITES PART B-ENGINEERING
·
2022
·
IF 11.322
Xinbin Wu,Wei Yu,Wei Xu,Yujun Zhang,Shundong Guan,Zheng Zhang,Shuwei Li,Huanchun Wang,Xuanjun Wang,Liang Zhang,Ce-Wen Nan,Liangliang Li
Lithium-oxygen (Li–O 2 ) batteries are promising next-generation energy storage devices due to their ultrahigh theoretical specific energy. Oxide electrocatalysts such as RuO 2 are often used to improve the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) processes in Li–O 2 batteries, but the relation between the structural parameters and their catalytic properties is unclear so far. In this work, we synthesize RuO 2 nanoparticles at different annealing temperatures and investigate the influence of the Ru–O bond distances of RuO 2 on the OER and ORR processes in Li–O 2 batteries. The results of X-ray absorption fine structure show that the bond distances decrease with the increase of the annealing temperature. The RuO 2 with longer Ru–O bond distances renders a lower charge plateau to Li–O 2 batteries, showing a better OER performance, while that with shorter bond distances gives a larger discharge capacity and is more friendly to the ORR process. The cycle life of Li–O 2 batteries with a carbon nanotube-RuO 2 composite cathode is improved to 287 cycles (1148 h) under an extreme testing condition (the voltage range is 2.3–4.2 V), when the Ru–O bond distances are optimized. In addition, the influence of the Ru–O bond distances on the catalytic properties of RuO 2 is analyzed by density functional theory calculations. The findings in this work provide a guidance to enhance the ORR and OER efficiency of RuO 2 and other oxide catalysts.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2023
·
IF 13.1
Rongrong Zhang,Beibei Guo,Lun Pan,Zhen-Feng Huang,Chengxiang Shi,Xiangwen Zhang,Ji-Jun Zou
Metal oxyhydroxides (MOOH) generated from irreversible reconstructions of transition metal compounds are intrinsic active species for oxygen evolution reaction , whose activities are still constrained by sluggish deprotonation kinetics and inherent adsorption energy scaling relations. Herein, we construct a tunable proton acceptor (TPA) on oxyhydroxides by in-situ reconstruction of metal oxoacids such as NiC 2 O 4 to accelerate deprotonation and break adsorption energy scaling relations during OER. The modified C 2 O 4 2− as a TPA can easily extract H of *OH (forming *HC 2 O 4 intermediate) and then promote deprotonation by the transmitted hydrogen bond with *OOH along conjugated (H···)O C–O(–H) chain. As a result, NiOOH-C 2 O 4 shows non-concerted proton-electron transfer and improved deprotonation rate, and delivers a good OER activity (270 mV@10 mA cm −2 ). The conjugate acidity coefficient (p K a ) of the modified oxoacid group can be a descriptor for TPA selection. This TPA strategy can be universally applied to Co-, Fe-, and Ni-based oxyhydroxides to facilitate OER efficiency.
研究领域:
材料科学
·
电化学
✓ 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）