APPLIED CATALYSIS B-ENVIRONMENTAL
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2022
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IF 24.319
Ting Wang,Fuli Sun,Shoujie Liu,Guilin Zhuang,Benxia Li
Supported Cu single-atom (Cu-SA) catalysts have exhibited unique activity and selectivity in CO 2 reduction, but they generally suffer from the easy transformation of active Cu δ+ into inactive Cu 0 . Herein, porous TiO 2 supported Cu single atoms (Cu-SAs/TiO 2 ) photocatalyst was fabricated and dioxygen (O 2 ) enhanced photocatalytic CO 2 reduction performance of Cu-SAs/TiO 2 was investigated by in-situ characterizations and theoretical calculations. The results showed that both activity and stability of Cu-SAs/TiO 2 photocatalyst could be improved by feeding a small amount of O 2 (117.6 ppm) in the reaction system. The competitive electron transfer to O 2 on Cu-SAs/TiO 2 maintained dynamic stability of Cu δ+ active sites, and O 2 -derived *OOH species lowered the formation energy barrier of key intermediate *COOH as well as delivered *H species for accelerating intermediates protonation process. Total yield rate of CH 4 and CO reached 34.64 μmol·g cat ·h −1 for CO 2 photoreduction over Cu-SAs/TiO 2 after introducing 117.6 ppm O 2 , accompanied by enhanced durability.
研究领域:
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
SENSORS AND ACTUATORS B-CHEMICAL
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2025
·
IF 7.7
Ying Qian,Jie Zou,Xiaoqing Jiang,Jie Wang,Juan Zhou,Chu Cheng,Xin Zhang,Wenming He,Qinghui Jin,Jiawen Jian
Yttria-stabilized zirconia (YSZ)-based amperometric humidity sensors are highly promising for in situ detection of high-temperature flue ducts due to their excellent stability and durability under extreme conditions. However, selectivity remains challenging due to the co-electrolysis of H 2 O and CO 2 , as these compounds have similar electrolysis voltages. In this study, LaFeO 3 is proposed as a sensing electrode to reduce CO 2 electrolysis and improve selectivity in amperometric humidity sensors. Analysis indicates that the improved selectivity is likely due to LaFeO 3 ’s lower electrochemical activity. Furthermore, the proposed sensor exhibits good repeatability and acceptable long-term stability for high-temperature humidity detection.
研究领域:
材料科学
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传感器技术
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jun Mou,Xingqi Fan,Fei Liu,Xiaodan Wang,Tianxiang Zhao,Peng Chen,Ziwei Li,Chunliang Yang,Jianxin Cao
The direct conversion of CO 2 hydrogenation to lower olefins via methanol as an intermediate is of great significance, but challenges still remain. Herein, we present a binary Mn 2 O 3 -ZnO oxide, which is responsible for catalytic hydrogenation of CO 2 to methanol. After combination of Mn 2 O 3 -ZnO and SAPO-34 molecular sieve, the catalytic reaction displays a markable increase. CO 2 adsorption by alkaline nature, followed by oxygen vacancy activation and synergistic hydrogenation over the binary Mn 2 O 3 -ZnO oxide are the prerequisites for the tandem reaction. However, the tandem spacing between oxide and molecular sieve plays a crucial role, because the suitable intimacy can induce enhanced methanol formation as intermediate via tandem dynamics effect, causing an apparent limitation for reverse water gas shift reaction at high temperature. The optimum mass ratio of 3:1 for two phases demonstrates that more components of binary oxide are needed to improve the rate of CO 2 hydrogenation to methanol, aiming to balance the two-step tandem reaction. Finally, under conditions of 380 ℃, 3 MPa and 3600 mL/g cat /h, 20%Mn 2 O 3 -ZnO/SAPO-34 tandem catalyst is obtained by physical ball milling after 15 min, with excellent stability, sulfur tolerance and catalytic performance with CO 2 conversion at almost 30%, lower olefins selectivity of 80.2% (propylene/ethylene = 5.6:1), and single-pass yield of 10.7%.
研究领域:
催化化学
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能源化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Xuandong Wang,Jie He,Liang Mao,Xiaoyan Cai,Chuanzhi Sun,Mingshan Zhu
Photocatalytic CO 2 conversion to valuable fossil fuels has been demonstrated to be a promising approach to reduce emissions of CO 2 and produce renewable energy, which primarily depends on developing the high efficiency of charge separation photocatalysts. Herein, CsPbBr 3 , one typical kind of all-inorganic perovskite nanocrystal, is immobilized on monolayer MoS 2 nanosheets to construct a new and ideal CsPbBr 3 /MoS 2 photocatalyst in the application of CO 2 photoreduction. In comparison with pure CsPbBr 3 , CsPbBr 3 /MoS 2 heterostructures possessed a specific electric field to more efficiently separate charges and generated more active sites for facilitating CO 2 activation, resulting in 3.0 and 2.4 times yields for CO 2 photoreduction to CH 4 and CO, respectively. Detailed characterization methods such as photoluminescence, surface photovoltage spectroscopy and theory calculations indicate the vivid illustrations of photogenerated carries separation which contributes to improving photocatalytic CO 2 conversion efficiency. The present investigation is anticipated to provide a new way for fabricating highly efficient perovskite-based photocatalyst in solar-energy-driven applications.
研究领域:
材料科学
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环境科学
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化学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2023
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IF 6.2
Ruijie Chen,Lei Wang,Jing Ding,Jinfeng Zhang,Hui Wan,Guofeng Guan
Photocatalytic CO 2 reduction can simultaneously alleviate the energy crisis and solve environmental issues. Nevertheless, it is still challenging for designing photocatalysts with efficient carrier mobility in rational. Herein, the Bi 2 MoO 6 /g-C 3 N 4 (BMO/CN) heterostructure was constructed through a microwave-assisted which could enhance the construction of two-dimensional and two-dimensional (2D/2D) structures. The 2D/2D BMO/CN heterojunction possessed excellent charge separation efficiency which exhibited superior performance on photocatalytic CO 2 reduction. It was shown by the characterization that the (131) surface of Bi 2 MoO 6 was constructed with the (100) surface of g-C 3 N 4 . The work functions of Bi 2 MoO 6 and g-C 3 N 4 were determined to be 4.57 and 4.22 eV, respectively, which suggested the type-II heterojunction was formed. The formation of CO and CH 3 OH over the optimized BMO/CN-30% catalyst reached 2.44 and 3.61 µmol⋅g −1 ⋅h −1 , respectively. The immediate products of HCO 3 - were observed within in-situ FT-IR to further certify the evolution of CH 3 OH. This work highlighted a microwave-assisted strategy to build a heterojunction structure for enhancing photoreduction CO 2 .
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2023
·Vol. 13
·期 6
·1830-1845
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IF 5
Hong Wang,Zhongming Wang,Mingquan Xiao,Zizhong Zhang,Xianzhi Fu,Wenxin Dai
Improving product selectivity is the most important goal for the artificial photosynthesis of CO2 and H2O considering that the adsorption behaviors of reactants may play an important role in the product selectivity of CO2 conversion. In this work, a black In2O3 sample was modified with fluoride anions (F−) as electron donors or amino ions (NH2+) as electron acceptors. F-modified In2O3 provided additional F− and In2+ sites, which promoted H2O to accept more electrons from the material, and exhibited a high selectivity to CH4 of 81.95%. NH2-modified In2O3 caused H2O to donate electrons to the material by constructing a hydrophobic layer, resulting in a high combined selectivity to methanol and carbon monoxide of 87.64%. Based on the two different H2O adsorption behaviors at In2+ sites adjacent to oxygen vacancy defects (VO–In2+) or at In3+ sites, the respective formation of hydrogen ions (H+) or protons (*H) is key to regulating the product selectivity of CO2 reduction. The formation of a confined-space structure of CO2 and its capacity to accept more electrons from the material induced by a higher number of VO–In2+ sites after modification both ensure the proceeding of CO2 reduction. The findings presented in this work add to the understanding of artificial photosynthesis.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2020
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IF 5.774
Minmin Gou,Weifang Zhu,Yanyong Sun,Ruili Guo
Two-dimensional (2D) MOF named Cu(BPY) 2 (OTF) 2 (OTF = trifluoromethanesulfonic acid anion (CF 3 SO 3 − ), BPY = 4,4-bipyridine) possessing axial coordination anion was prepared, and then combined into Pebax® MH 1657 (Pebax) polymer to fabricate mixed matrix membranes (MMMs) for the separation of CO 2 /CH 4 gas mixtures. The inherent microporous structure and interlayer nanochannel that constructed by axial coordination anion CF 3 SO 3 − of Cu(BPY) 2 (OTF) 2 nanosheets provide selective transfer channels for CO 2 . In addition, the group that has an affinity for CO 2 , such as pyridine group and CF 3 SO 3 − anion, locating in the surface and the interlayer of Cu(BPY) 2 (OTF) 2 nanosheets, present better binding affinity and molecule selectivity for CO 2 . Owing to the synergistic effect between structure and functional groups of Cu(BPY) 2 (OTF) 2 nanosheets, the optimized CO 2 separation performance (permeability and selectivity) of the MMMs compared with that of pure Pebax were increased by 86.65% and 47.59%, respectively, under the conditions of pure gas, 0.1 MPa and 25 °C. The open narrow nanochannels and axial coordination anion in Cu(BPY) 2 (OTF) 2 nanosheet, making Cu(BPY) 2 (OTF) 2 a promising material to prepare efficient mixed matrix membrane.
研究领域:
材料科学
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化学工程
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
International Journal of Greenhouse Gas Control
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2019
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IF 3.231
Mimi Xu,Shujuan Wang,Lizhen Xu
21 pairs of physical-chemical biphasic solvents were screened out using a fast screening facility and the distribution of components was detected both in upper and lower phases after absorption. The physical solvents and amines were enriched in opposite phases due to the limited solubility of absorption products in the physical solvents, and the enrichment of components gets higher as the loading time goes by. Comparisons of the cyclic capacity showed that MEA and DETA were much better main solvents than BDA in biphasic solvents, and 2.5 DETA-4 sulfolane has the highest CO 2 cyclic capacity of 4.486 mol L −1 , which was much higher than that of 30 wt% MEA. The concentrations of physical solvents influence the cyclic capacity a lot rather than the types of physical solvents. Then the phase separation character and absorption performance were analyzed for solutions in different amine to physical solvent concentration ratios, and the results showed that increasing the concentration of the physical solvent within certain range benefits to raising cyclic absorption capacity and reducing the energy penalty. At last, the sensible heat and vaporization heat of two biphasic solvents were estimated with a flash module of Aspen Plus, which showed less energy penalty than that of 30 wt% MEA.
研究领域:
化学工程
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环境科学
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DOI
高影响因子
Jove-Journal of Visualized Experiments
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2019
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IF 1.108
XiaoXiang Fang,Zhihong Gao,Hanfeng Lu,Qiulian Zhu,Zekai Zhang
We demonstrate a method for the enhancement of CO2 photoreduction. As the driving force of a photocatalytic reaction is from solar light, the basic idea is to use concentration technology to raise the incident solar light intensity. Concentrating a large-area light onto a small area cannot only increase light intensity, but also reduce the catalyst amount, as well as the reactor volume, and increase the surface temperature. The concentration of light can be realized by different devices. In this manuscript, it is realized by a Fresnel lens. The light penetrates the lens and is concentrated on a disc-shaped catalyst. The results show that both the reaction rate and the total yield are efficiently increased. The method can be applied to most CO2 photoreduction catalysts, as well as to similar reactions with a low reaction rate at natural light.
研究领域:
环境科学
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能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yingying Cai,Aikelaimu Aihemaiti,Yiping Su,Yongqi Sun,Xin Sun,Heng Li,Kezhen Chen,Xuehua Shen,Feng Yan,Fan Qu,Heijin Chen,Zuotai Zhang
In this study, the CO 2 -looping system was firstly attempted to build for exploring the effect of calcium-based (Ca-based) additives on pyrolytic characteristics and products in co-pyrolysis of sewage sludge (SS) and biomass. Then, an innovation method for the consumption of CO 2 (CP CO2 ) evaluation was proposed and carried out in the CO 2 -looping system, in which it was evaluated based on the syngas volume and CO 2 proportion. The results revealed that the addition of CaO and Ca(OH) 2 could significantly improve CP CO2 by 21.2% in the co-pyrolysis of 500 ℃, while the CaCO 3 addition decreased the CP CO2 by 1.0%. Besides, the co-pyrolysis temperature more than 700 ℃ would play more significant role on the CP CO2 than the addition of Ca-based additives. Then the effect of Ca-based types on biochar characteristics was also identified accompanied by the bio-oil composition. Results showed that the CaO and Ca(OH) 2 additives not only increased biochar mass and pH, but also enhanced the dissolved organic carbon content and the variety of dissolved organic matter, and reduced the total HMs content. Meanwhile, it was 15 types of components that was identified in bio-oil by NIST mass spectral library, found that the intensity of heptadecanenitrile and estra-1,3,5(10)-trien-17 beta-ol was influenced by Ca-based additives. Moreover, the CaO and Ca(OH) 2 played important roles for improving the CP CO2 in the CO 2 -looping system, which was further verified by Fact Sage. Finally, the mechanism for the Ca-based additives on CP CO2 was proposed at different co-pyrolysis temperatures. These findings can widen paths for biochar application and development of CO 2 capture materials.
研究领域:
环境科学
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化学工程
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能源工程
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 31
·15064-15073
·
IF 9.931
Xu Jiang,Songwei Li,Shanshan He,Yongping Bai,Lu Shao
Both material choice and filler/organic interface are crucial in mixed matrix membranes (MMMs) for sub-nano-size gas separations and yet, the interface–performance relationship is still a subject of intense debate due to challenging interfacial detection. Herein, two UiO-66-type MOFs (amino-functionalized UiO-66-NH2 and isopropenyl-functionalized UiO-66-MA) are incorporated in cross-linked CO2–philic polyethylene oxide (PEO) matrix based on judicious material screening for CO2 capture. The reactive material UiO-66-MA is stitched together with methacrylate-capped PEO in situ during UV-induced copolymerization to generate highly efficient gas transport passages with conceivably good interfaces. Poor interface is observed by substituting UiO-66-MA with non-reactive UiO-66-NH2 in MPCM (MOF/polymer composite membrane). The interfacial conditions of CO2–philic MPCMs are carefully assessed via advanced physicochemical characterizations for clarifying the correlation between interface and separation performance. The reactive material UiO-66-MA containing MPCM with good interface demonstrates higher gas permeability (up to 1450 barrers) with similar selectivity (up to 45.8 for CO2/N2) when compared to non-reactive UiO-66-NH2 containing MPCM. The mixed gas test also shows high CO2 permeability of 1439 barrer and CO2/N2 selectivity of 37.6 in our MPCM. We also observe unexpected suppressed plasticization/swelling behaviour in UiO-66-MA containing MPCM and enhanced plasticization in UiO-66-NH2 containing MPCM through analysis of gas separation performance in the range of 1–10 atm, which might be utilized as a potential interface assessment tool for nanocomposites. Moreover, the performances of our CO2–philic MPCMs can be optimized further to surpass the (2008) Robeson Upper Bound for highly efficient sustainable CO2 capture.
研究领域:
材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Nana Zhou,Yurong Yin,Baojuan Luo,Yongxin Fu,Xiaoxun Ma,Chengyi Dai
The electrochemical CO 2 reduction reaction (eCO 2 RR), which is well suited for reducing atmospheric CO 2 levels and generating clean energy. Water is the main proton source in the electrochemical reduction process. However, water features a high dissociation energy barrier, and most protons are involved in HER, so that only a small amount of H + is used in the CO 2 reduction reaction. Herein, we reveal that appropriately chosen ligands on the catalyst surface can abstract protons from water, store them, and transfer them to CO 2 to promote the formation of COOH and improve the proton utilization efficiency of the eCO 2 RR. Moreover, the activity of the ligand complexed protons is shown to be lower than that of free ones and thus result in HER inhibition our ligands with different pK a values (i.e., proton release capacities) are used to functionalize ZnO, and the plot of pK a vs. the FE CO exhibits a volcano shape. Overly small pK a leads to the combination of abundant protons with each other and the dominance of the HER, whereas overly large pK a does not promote the utilization of H + by CO 2 . Ligands with suitable pK a can properly bind and release protons, which is conducive to the formation of *COOH, thus accelerating eCO 2 RR. In particular, mercaptobenzoic acid (MBA) considerably enhances catalytic activity because of its moderate pK a (FE CO = 90 %, which is 2 times higher than the FE CO of unmodified ZnO, and j CO is nearly 5 times higher). In situ infrared spectroscopic analysis proves that the above ligand can abstract protons from H 2 O and then release them, promoting the dissociation of H 2 O. Theoretical calculations show that pK a affects the ability of ligands to abstract and release protons.
研究领域:
材料科学
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电化学
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催化反应
✓ 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）