ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Yongping Gan,Min Huang,Fei Yu,Xing Yu,Zhanjun He,Jin Liu,Tiejun Lin,Yuanyuan Dai,Qiang Niu,Liangshu Zhong
Light-driven methane conversion to methanol with high selectivity is considered a challenging and promising reaction for sustainable development. Herein, Cu/CeO2 catalysts were prepared for photocatalytic methane conversion with CO2 as a soft oxidant. Methanol was the sole liquid product with a high selectivity of 96.2% and a high yield of 88.9 μmol g–1 h–1 for the 2Cu/CeO2 catalyst. Investigation of the structure–performance relationship indicated that oxygen vacancies facilitated the trapping of photogenerated electrons and avoided carrier recombination. In addition, as a soft oxidant, CO2 can also capture photogenerated electrons to be reduced to CO and further accelerate the formation of CH3OH. A catalytic mechanism study demonstrated that methane and hydroxyl were oxidized by photogenerated holes to •CH3 and •OH, respectively, and thus, methanol was generated through the combination of •CH3 and •OH.
研究领域:
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
高影响因子
Materials Today Energy
·
2021
·
IF 7.311
Lina Yan,Xing Cheng,Yueshuai Wang,Zhaozhao Wang,Lirong Zheng,Yong Yan,Yue Lu,Shaorui Sun,Wenge Qiu,Ge Chen
The electrochemical production of hydrogen peroxide via the two-electron (2e − ) oxygen reduction reaction (ORR) is an environmentally friendly method and is expected to be an alternative means to the industrial anthraquinone process. It is particularly suitable for on-site and small-scale H 2 O 2 requirements. The development of earth-abundant catalysts with high activity and selectivity toward H 2 O 2 is highly desirable and challenging. Here, we have prepared Co 3 O 4 with tunable oxygen vacancies (OVs) and strongly coupled it to nitrogen-doped carbon nanotubes through an exsolution strategy. The Co 3 O 4 with a higher OV concentration exhibits a higher 2e − ORR activity, higher H 2 O 2 selectivity, and lower H 2 O 2 reduction reaction (H 2 O 2 RR) activity so that effectively improving the production rate of H 2 O 2 (1.6 mol peroxide/g catalyst /h at 0.0 V RHE ) in acidic media. The catalyst is also used as a cathode for the electro-Fenton process and degrades up to 80% of 40 mg/L of rhodamine B solution within 25 min. Density functional theory calculation shows that the ∗ OOH binding energy (Δ G ∗OOH ) could decrease on increasing the numbers of OVs, which subsequently benefits the protonation of ∗ OOH to generate H 2 O 2 .
研究领域:
材料科学
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电化学
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环境科学
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产品关联
DOI
高影响因子
BMC MICROBIOLOGY
·
2016
·Vol. 16
·期 1
·1-11
·
IF 2.581
Wang Dan,Zhu Fengqiu,Wang Qian,Rensing Christopher,Yu Peng,Gong Jing,Wang Gejiao
Background Microbial antimonite [Sb(III)] oxidation converts toxic Sb(III) into less toxic antimonate [Sb(V)] and plays an important role in the biogeochemical Sb cycle. Currently, little is known about the mechanisms underlying bacterial Sb(III) resistance and oxidation. Results In this study, Tn5 transposon mutagenesis was conducted in the Sb(III)-oxidizing strain Pseudomonas stutzeri TS44 to isolate the genes responsible for Sb(III) resistance and oxidation. An insertion mutation into gshA, encoding a glutamate cysteine ligase involved in glutathione biosynthesis, generated a strain called P. stutzeri TS44-gshA 540 . This mutant strain was complemented with a plasmid carrying gshA to generate strain P. stutzeri TS44-gshA-C. The transcription of gshA , the two superoxide dismutase (SOD)-encoding genes sodB and sodC as well as the catalase-encoding gene katE was monitored because gshA -encoded glutamate cysteine ligase is responsible for the biosynthesis of glutathione (GSH) and involved in the cellular stress defense system as are superoxide dismutase and catalase responsible for the conversion of ROS. In addition, the cellular content of total ROS and in particular H 2 O 2 was analyzed. Compared to the wild type P. stutzeri TS44 and TS44-gshA-C, the mutant P. stutzeri TS44-gshA 540 had a lower GSH content and exhibited an increased content of total ROS and H 2 O 2 and increased the Sb(III) oxidation rate. Furthermore, the transcription of sodB , sodC and katE was induced by Sb(III). A positive linear correlation was found between the Sb(III) oxidation rate and the H 2 O 2 content ( R
2 = 0.97), indicating that the accumulated H 2 O 2 is correlated to the increased Sb(III) oxidation rate. Conclusions Based on the results, we propose that a disruption of the pathway involved in ROS-protection allowed H 2 O 2 to accumulate. In addition to the previously reported enzyme mediated Sb(III) oxidation, the mechanism of bacterial oxidation of Sb(III) to Sb(V) includes a non-enzymatic mediated step using H 2 O 2 as the oxidant.
研究领域:
微生物学
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环境科学
✓ 已验证
DOI
PubMed
高影响因子
Energy Technology
·
2018
·Vol. 7
·期 3
·1800747
·
IF 3.175
Pengjing Chen,Longang Tao,Jian Zhu,Guofeng Zhao,Ye Liu,Yong Lu
Indium oxide is as a promising catalyst for the hydrogenation of CO 2 to methanol. Previous studies mainly focused on the cubic-phase In 2 O 3 (C-In 2 O 3 ), but the hexagonal-phase In 2 O 3 (H-In 2 O 3 ) with a corundum structure has been rarely studied because of the difficulty in its synthesis. Herein, the morphology-controllable H-In 2 O 3 in situ structured onto a thin-felt Al 2 O 3 /Al-fiber is prepared by a facile mixed solvothermal method. The amount of H-In 2 O 3 is strongly dependent on the urea/In molar ratio during the mixed solvothermal synthesis. The optimal catalyst obtained at a urea/In ratio of 4.5 possesses the highest amounts of oxygen vacancy and strong basic site. Such catalyst achieves a turnover frequency of 47.8 h −1 (the number of CO 2 converted into methanol per oxygen vacancy site per hour) and is stable for at least 200 h, being capable of converting 4.4% CO 2 into methanol at a selectivity of 67.6% at 325 °C (or higher selectivity at the expense of conversion below 325 °C) with a methanol space time yield of 0.20 g MeOH g cat −1 h −1 . In contrast, the microfibrous-structured C-In 2 O 3 (prepared by the incipient wetness impregnation method) delivers a very low methanol selectivity of only 36.8% under identical reaction conditions. In situ Fourier transform infrared spectroscopy experiments reveal that the H-In 2 O 3 /Al 2 O 3 /Al-fiber catalyzes CO 2 -to-methanol conversion through formate intermediates.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
EUROPEAN JOURNAL OF LIPID SCIENCE AND TECHNOLOGY
·
2018
·Vol. 121
·期 4
·1800078
·
IF 2.2
Xue Li,Ruinan Yang,Chunling Lv,Lin Chen,Liangxiao Zhang,Xiaoxia Ding,Wen Zhang,Qi Zhang,Chundi Hu,Peiwu Li
The residues of chlorophyll induce oxidative rancidity and deterioration through photo-oxidation. However, the effect of chlorophyll on the quality of rapeseed oil is still unknown. In this study, chlorophyll is added into rapeseed oil to reach the desired treatment levels of 2, 5, and 10 mg kg −1 , while no chlorophyll is added in the control sample. Dynamic changes of the peroxide value of rapeseed oils with different chlorophyll contents exposed to light and stored in the dark at different times (0, 1, 5, 10, 15, 20, 25, 30, 35, 40, 45, 50, 55, and 60 days) are investigated. The results show that the peroxide value of rapeseed oil exposed to light increased significantly, especially for the oil with a high content of chlorophyll. In contrast, the peroxide value of rapeseed oil stored in the dark is nearly unchanged no matter whether extra chlorophyll is added. This study shows that chlorophyll in rapeseed oil can trigger oil oxidation, and therefore it is necessary to take measures to reduce the chlorophyll content in rapeseed oil or store rapeseed oil in the dark as soon as possible. Practical Applications : This study shows that chlorophyll in rapeseed oil can trigger oil oxidation, and therefore it is necessary to take measures to reduce the chlorophyll content in rapeseed oil. In this study, dynamic changes of peroxide values of rapeseed oils with different chlorophyll contents exposed to light and stored in the dark at different times are investigated. The results show that the peroxide value of rapeseed oil exposed to light increases significantly, especially for the rapeseed oil with a high content of chlorophyll. In conclusion, chlorophyll in rapeseed oil can trigger oil oxidation.Therefore, it is necessary to take measures to reduce the chlorophyll content in rapeseed oil or store rapeseed oil in the dark as soon as possible.
研究领域:
食品科学
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植物化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2020
·
IF 7.489
Fukun Bi,Xiaodong Zhang,Shang Xiang,Yunyun Wang
The effect of Pd loading (0.25, 0.5 and 1.0 wt%) and ZrO 2 support calcined at diverse temperatures (600, 700 and 800 °C) by pyrolysis of UiO-66 was investigated for CO oxidation in this work, respectively. The physicochemical properties of the samples were characterized by various characterization methods. The XRD results exhibited that all ZrO 2 support possessed mixed crystalline phase, the monoclinic ZrO 2 and tetragonal ZrO 2 . And the calcination temperature had a big impact on the composition of ZrO 2 supports. Pyrolysis of UiO-66 at high temperature was favorable for the formation of monoclinic ZrO 2 . Additionally, the introduction of Pd was induced the phase conversion from tetragonal to monoclinic of ZrO 2 . The order of catalytic efficiency was as follows: 0.5Pd/Zr-700 > 0.5Pd/Zr-600 > 0.5Pd/Zr-800. Moreover, 0.5Pd/Zr-700 presented high stability and great reusability. The good catalytic performance of 0.5Pd/Zr-700 was ascribed to the better reduction ability at low temperature and high O ads /O lat and Pd 0 /Pd 2+ on the surface. Importantly, the reaction pathway of CO oxidation over the 0.5Pd/Zr-700 was exposed.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Fang Peng,Weiwei Yu,Yue Lu,Yan Sun,Xiuli Fu,Jia ming Hao,Xin Chen,Rui Cong,Ning Dai
To verify the effect of oxygen vacancy on gas sensitivity, we have systematically investigated the gas-sensing performance of copper oxide/substoichiometric tungsten oxide (CuO/WO3–x) nanocomposite sensors. Oxygen deficiency in WO3–x facilitates the reaction of hydrogen sulfide (H2S) gas with chemisorbed oxygen species (i.e., O2–, O–, and O2–) at low temperature. The oxygen/sulphur exchange reaction between CuO and H2S in the sensing process can achieve room temperature operation of gas sensors. After the WO3–x nanorods were modified by a low content of CuO nanoparticles (Cu:W = 1:20), the sensors present an n-type sensing behavior. Their best working temperatures drop from 289 °C (or 386 °C) to 99 °C (or 70 °C) at which the responses are improved by 14 to 163 times for different x values. Among them, CuO(L)/W5O14 shows the highest sensitivity of 1575.7 to 10 ppm H2S at 99 °C and 171.5 to 10 ppm H2S at room temperature. Once WO3–x were loaded with a high concentration of CuO nanoparticles (Cu:W = 1:2), they exhibit a p-type behavior, and the optimal working temperatures reduce suddenly to room temperature at which CuO(H)/W18O49 displays the most sensitive response of 7.2 even toward trace amounts of H2S as low as 100 ppb. In addition, p-type CuO weakens the metal-like characteristics of W18O49 and such weakening effect enhances with an increase in the CuO content. Therefore, the sensing performance of the CuO/W18O49 composite is the best among the four CuO/WO3–x sensors. The two designs for low and high Cu/W molar ratios all achieve enhanced room-temperature H2S gas response, with a fast recovery time of ∼60 s under heating pulse, as well as an excellent selectivity, which makes the sensors a promising candidate for practical applications. Moreover, the micro-Raman spectra confirmed CuS formation and the thermal effect on the decomposition of CuS in the sensing process was studied.
研究领域:
材料科学
·
传感器技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 8
·2392-2403
·
IF 4
Amir Said,Guanyun Zhang,Caiyun Liu,Dexin Wang,Huihui Niu,Yanshu Liu,Guanjie Chen,Chen-Ho Tung,Yifeng Wang
The cycloaddition reaction of CO2 to epoxides is quite promising for CO2 capture and storage as well as the production of value-added fine chemicals. Herein, a novel atomically precise lead-doped titanium-oxide cluster with the formula Ti10Pb2O16(phen)4(Ac)12(DMF)2 (denoted as Ti10Pb2; phen = 1,10-phenanthroline; Ac = acetate; DMF = dimethylformamide) was synthesized through a facile solvothermal process, and is a molecular photocatalyst with surface-anchored main-group metal active sites. Its structure was characterized by single-crystal X-ray diffraction and other complementary techniques. Ti10Pb2 showed high photo-response and charge-separation efficiency under simulated sunlight irradiation. Ti10Pb2 was successfully used in the cycloaddition reaction of CO2 with epoxides under solvent-free conditions. While its catalytic activity due to the Lewis acidity was moderate, simulated solar light irradiation further enhanced the reaction rate, demonstrating the synergistic effect of photocatalysis and Lewis-acid thermocatalysis.
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Lei Wang,Yonggang Sun,Yulong Ma,Min Xu,Juan Zhang,Yingbo Zhu,Jie Ding,Li Zhu,Jing Ma,Wenxin Ji,Liqiong Wang,Yuanyuan Li
Dual activation of molecular and lattice oxygen is an important step in the catalytic oxidation of volatile organic compounds. Herein, CeO 2 was derived from MOF as an electron donor support to develop a co-catalyst with Pt-Pd alloy nanoparticles (Pt-Pd/CeO 2 ). The Prepared Pt-Pd/CeO 2 exhibits excellent catalytic activity towards toluene oxidation, showing a turnover frequency (TOF 0.26 s −1 ) higher than those of Pt/CeO 2 (0.05 s −1 ) and Pd/CeO 2 (0.02 s −1 ). Several in situ experimental techniques and density functional theory calculations have revealed that the introduction of Pd valence electrons can intensify the electronic metal-support interactions (EMSIs) effects of Pt-Pd/CeO 2 catalysts, which can weaken the Ce-O bond, thereby promoting the production and circulation of lattice oxygen and oxygen vacancies, and modulating the d -band centre to enhance the adsorption and activation of reactants. This study presents a comprehensive investigation of toluene oxidation on alloy-supported catalysts, providing practical guidance for designing reliable catalysts suitable for industrial applications.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2023
·
IF 12.8
Chaoyun Ying,Chang Liu,Feng Zhang,Lirong Zheng,Xiaoming Wang,Hui Yin,Wenfeng Tan,Xionghan Feng,Bruno Lanson
Manganese (Mn) oxides are extensively used to oxidize As(III) present in ground, drinking, and waste waters to the less toxic and more easily removable As(V). The common presence of multiple other cations in natural waters, and more especially of redox-sensitive ones such as Fe 2+ , may however significantly hamper As(III) oxidation and its subsequent removal. The present work investigates experimentally the influence of Mn(III) chelating agents on As(III) oxidation process in such environmentally relevant complex systems. Specifically, the influence of sodium pyrophosphate (PP), an efficient Mn(III) chelating agent, on As(III) oxidation by birnessite in the presence of Fe(II) was investigated using batch experiments at circum-neutral pH. In the absence of PP, competitive oxidation of Fe(II) and As(III) leads to Mn oxide surface passivation by Fe(III) and Mn(II/III) (oxyhydr)oxides, thus inhibiting As(III) oxidation. Addition of PP to the system highly enhances As(III) oxidation by birnessite even in the presence of Fe(II). PP presence prevents passivation of Mn oxide surfaces keeping As and Fe species in solution while lower valence Mn species are released to solution. In addition, reactive oxygen species (ROS), tentatively identified as hydroxyl radicals (•OH), are generated under aerobic conditions through oxygen activation by Fe(II)–PP complexes, enhancing As(III) oxidation further. The positive influence of Mn(III) chelating agents on As(III) oxidation most likely not only depend on their affinity for Mn(III) but also on their ability to promote formation of these active radical species. Finally, removal of As(V) through sorption to Fe (oxyhydr)oxides is efficient even in the presence of significant concentrations of PP, and addition of such Mn(III) chelating agents thus appears as an efficient way to enhance the oxidizing activity of birnessite in large-scale treatment for arsenic detoxification of groundwaters.
研究领域:
环境科学
·
化学
·
水处理工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yunshuo Zhu,Lili Guan,Xiwen Song,Yarong Huang,Ming Li,Qingxian Zhang,Ruihua Guo
Strict control of carbon emissions is crucial for expediting the achievement of carbon neutrality. However, the current CO 2 RR electrocatalytic exhibits numerous shortcomings that impede the enhancement of catalytic activity. Issues such as lengthy catalyst preparation times, and high levels of precious metal content. Additionally, the aggregation of ultrafine nanoparticles contributes to a rapid deterioration in catalytic performance. Herein, a Joule-heating method is efficiently utilized to synthesize heterostructures nano-catalysts for CO 2 electroreduction on carbon cloth substrates. This method takes advantage of the thermoelectric coupling of the carbon cloth to achieve carbothermal reduction, while also regulating phase composition and introduction of oxygen vacancies. The Cu-CeO 2 /TiO 2 /CC catalyst synthesized in this method showed a current density in CO 2 of −32 mA·cm −2 at −1.0 V (vs. RHE). Notably, this catalyst demonstrated high CO selectivity and Faraday efficiency (FE CO ) of up to 82.5 % at a low potential of −0.3 V (vs. RHE). Optimal electrochemical performance is achieved at a power of 40 W. The ultra-fast temperature change process prevented the agglomeration of catalyst particles and facilitated the construction of a stable heterogeneous interface with a high oxygen vacancy concentration. In conclusion, this study presents a promising approach, particularly for the rapid preparation of low-cost, highly selective non-precious metal electrocatalysts.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Small
·
2024
·
IF 13
Nan Wang,Tingxue Fang,Tinghui An,Yuhao Wang,Jiaqi Li,Shuming Yu,Honghai Sun,Dong Xiang,Xiangjie Bo,Kedi Cai
Li-O 2 batteries urgently needs high discharge capacity and stable cycling performance, requiring effective and reliable bifunctional catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Herein, Hovenia acerba Lindl -like heterostructure composed of cobalt sulfide and tin dioxide supported on carbon substrate (CoS/SnO 2 @C) is prepared via CO 2 laser irradiation technology. The half-wave potential of CoS/SnO 2 @C for the ORR is 0.88 V, while the overpotential of the OER at 10 mA cm −2 is as low as 270 mV. The Li-O 2 batteries employing the bifunctional CoS/SnO 2 @C catalyst displays a high discharge specific capacity of 3332.25 mAh g −1 and long cycling life of 226 cycles. Additionally, theory calculations demonstrate that the construction of heterostructure decreases energy barrier of the rate-determining step (RDS) for both ORR and OER. Notably, SnO 2 behaves as the electronic promoter to optimize the electronic structure of heterostructure interface and triggers charge redistribution of CoS, which weakens the adsorption strength of the * O-intermediates and allows to break the linear scaling relationship, thus further enhancing the catalytic performance of CoS/SnO 2 @C. This research furnishes directions for the design of heterogeneous catalysts, highlighting its great potential for application in rechargeable Li-O 2 batteries.
研究领域:
材料科学
·
电化学
·
能源存储与转换
✓ 已验证
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）