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学者姓名：陈标华
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摘要 ：
Poly(oxymethylene) dimethyl ethers (PODEn) is a promising excellent additive for diesel fuels. The PODEn production by traditional reactor conform to Schulz - Flory distribution resulting in low product yield and large circulating material flow, which leads to high energy consumption and cost. This study presents a novel reactive distillation (RD) process for the PODEn synthesis by polymerization reaction from trioxane and methylal. A rigorous simulation model of the RD process was developed for the plant design and scale-up. Also, a sensitivity analysis was performed to determine the influence of key operating parameters on the RD process performance. The production composition analysis indicates that the RD process can effectively control the degree of polymerization and obtain high selectivity for any target product(s). The techno-economic analysis shows that the process is feasible, with over 96% and 13% reduction in CapEx and OpEx, over 68% savings in total annual costs as compared to the reaction-separation technology. Higher conversion and selectivity can be obtained by RD, within lower recirculation rate (only 12281 kg/h instead of 2950 kg/h) as compared to the conventional process.
关键词 ：
Methylal Methylal PODEn PODEn Process design Process design Process intensification Process intensification Reactive distillation Reactive distillation
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| GB/T 7714 | Meng, Ying , Li, Hong , Dai, Chengna et al. Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 278 . |
| MLA | Meng, Ying et al. "Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane" . | SEPARATION AND PURIFICATION TECHNOLOGY 278 (2022) . |
| APA | Meng, Ying , Li, Hong , Dai, Chengna , Chen, Biaohua , Lei, Zhigang , Li, Xingang et al. Innovative reactive distillation process for the eco-friendly Poly (oxymethylene) dimethyl ethers synthesis from methylal and trioxane . | SEPARATION AND PURIFICATION TECHNOLOGY , 2022 , 278 . |
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摘要 ：
Next-generation desalination technologies are needed to meet the increasing demand for clean water. Capacitive deionization (CDI) is a thermodynamically efficient technique to treat non-potable water with relatively low salinity. The salt removal capacity and rate of CDI are highly dependent on the electrode materials, which are preferentially porous to store ions through electrosorption and/or redox reactions. Metal-organic frameworks (MOFs) with "infinite" combinations of transition metals and organic linkers simplify the production of carbonaceous materials often with redox-active components after pyrolysis. MOFs-derived materials show great tunability in both compositions and structures but require further refinement to improve CDI performance. This review article summarizes recent progress in derivatives of MOFs and MOF-like materials used as CDI electrodes, focusing on the structural and compositional material considerations as well as the processing parameters and electrode architectures of the device. Furthermore, the challenges and opportunities associated with this research area are also discussed.
关键词 ：
brackish water brackish water capacitive deionization capacitive deionization desalination desalination metal-organic frameworks metal-organic frameworks pyrolysis pyrolysis
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| GB/T 7714 | Wang, Hao , Chen, Biaohua , Liu, Di-Jia et al. Nanoarchitectonics of Metal-Organic Frameworks for Capacitive Deionization via Controlled Pyrolyzed Approaches [J]. | SMALL , 2021 . |
| MLA | Wang, Hao et al. "Nanoarchitectonics of Metal-Organic Frameworks for Capacitive Deionization via Controlled Pyrolyzed Approaches" . | SMALL (2021) . |
| APA | Wang, Hao , Chen, Biaohua , Liu, Di-Jia , Xu, Xingtao , Osmieri, Luigi , Yamauchi, Yusuke . Nanoarchitectonics of Metal-Organic Frameworks for Capacitive Deionization via Controlled Pyrolyzed Approaches . | SMALL , 2021 . |
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摘要 ：
Cobalt catalysts have great potentials towards CO hydrogenation. Herein, a facial H-2 pressure-controlled strategy was developed to synthesize two typical branched cobalt nanostructures: nail-like cobalt and urchin-like cobalt. The H-2-controlled over-growth mechanisms have been proposed, and supported by both experiments and DFT calculations. The over-growth of Co nanocrystals can be finely controlled by the selective and competitive adsorption between H-2 and OAm molecules on cobalt surface. Both nail-like cobalt and urchin-like cobalt exhibit superior CO hydrogenation activity to ordinary Co nanoparticles, due to their HCP phase, unique branch structure with high specific area, and more exposed active (1 0 -1 1) crystal facets.
关键词 ：
Branched structure Branched structure CO hydrogenations CO hydrogenations H-2-controlled overgrowth H-2-controlled overgrowth HCP cobalt (10-11) facets HCP cobalt (10-11) facets Phase and facets effects Phase and facets effects
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| GB/T 7714 | Zhang, Qinwei , Chen, Biaohua , Liang, Xin . Controlled over-growth for nail-like and urchin-like cobalt with enhanced CO hydrogenation activity [J]. | APPLIED SURFACE SCIENCE , 2021 , 537 . |
| MLA | Zhang, Qinwei et al. "Controlled over-growth for nail-like and urchin-like cobalt with enhanced CO hydrogenation activity" . | APPLIED SURFACE SCIENCE 537 (2021) . |
| APA | Zhang, Qinwei , Chen, Biaohua , Liang, Xin . Controlled over-growth for nail-like and urchin-like cobalt with enhanced CO hydrogenation activity . | APPLIED SURFACE SCIENCE , 2021 , 537 . |
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摘要 ：
This study proposes the capture of dimethyl sulfide (DMS) and dimethyl disulfide (DMDS) from waste gas using an ionic liquid (IL), namely, 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide ([EMIM][Tf2N]), and examines the process from a molecular level to the laboratory scale, which is then scaled up to the industrial level. The binding energy and weak interactions between DMS/DMDS and the anion/cation in [EMIM][Tf2N] were investigated using quantum chemistry calculations to identify the capture mechanism at the molecular scale. A thermodynamic model (UNIFAC-Lei) was established by the vapor−liquid equilibrium data of the [EMIM][Tf2N] + DMS/DMDS systems measured at the laboratory scale. The equilibrium and continuous absorption experiments were performed, and the results demonstrated that [EMIM][Tf2N] exhibits a highly efficient capture performance at atmospheric conditions, particularly, absorption capacities (AC) for DMS and DMDS are 189.72 and 212.94 mg g−1, respectively, and partial coefficients (PC) as more reasonable evaluation metrics for those are 0.509 × 10-4 and 6.977 × 10-4 mol kg−1 Pa−1, respectively, at the 100 % breakthrough. Finally, a mathematical model of the strict equilibrium stage was established for process simulations, and the absorption process was conceptually designed at the industrial scale, which could provide a decision-making basis for chemical engineers and designers. © 2020 Elsevier B.V.
关键词 ：
Binding energy Binding energy Decision making Decision making Ionic liquids Ionic liquids Quantum chemistry Quantum chemistry Sulfur Sulfur Sulfur compounds Sulfur compounds
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| GB/T 7714 | Xu, Ruinian , Dai, Chengna , Mu, Mingli et al. Highly efficient capture of odorous sulfur-based VOCs by ionic liquids [J]. | Journal of Hazardous Materials , 2021 , 402 . |
| MLA | Xu, Ruinian et al. "Highly efficient capture of odorous sulfur-based VOCs by ionic liquids" . | Journal of Hazardous Materials 402 (2021) . |
| APA | Xu, Ruinian , Dai, Chengna , Mu, Mingli , Cheng, Jun , Lei, Zhigang , Wu, Bin et al. Highly efficient capture of odorous sulfur-based VOCs by ionic liquids . | Journal of Hazardous Materials , 2021 , 402 . |
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摘要 ：
Increasing demand for sustainable and clean energy is calling for the next-generation energy conversion and storage technologies such as fuel cells, water electrolyzers, CO2 /N2 reduction electrolyzers, metal-air batteries, etc. All these electrochemical processes involve oxygen electrocatalysis. Boosting the intrinsic activity and the active-site density through rational design of metal-organic frameworks (MOFs) and metal-organic gels (MOGs) as precursors represents a new approach toward improving oxygen electrocatalysis efficiency. MOFs/MOGs afford a broad selection of combinations between metal nodes and organic linkers and are known to produce electrocatalysts with high surface areas, variable porosity, and excellent activity after pyrolysis. Some recent studies on MOFs/MOGs for oxygen electrocatalysis and their new perspectives in synthesis, characterization, and performance are discussed. New insights on the structural and compositional design in MOF/MOG-derived oxygen electrocatalysts are summarized. Critical challenges and future research directions are also outlined.
关键词 ：
electrocatalysis electrocatalysis metal-organic frameworks metal-organic frameworks metal-organic gels metal-organic gels oxygen evolution reaction oxygen evolution reaction oxygen reduction reaction oxygen reduction reaction
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| GB/T 7714 | Wang Hao , Chen Biao-Hua , Liu Di-Jia . Metal-Organic Frameworks and Metal-Organic Gels for Oxygen Electrocatalysis: Structural and Compositional Considerations. [J]. | Advanced materials , 2021 : e2008023 . |
| MLA | Wang Hao et al. "Metal-Organic Frameworks and Metal-Organic Gels for Oxygen Electrocatalysis: Structural and Compositional Considerations." . | Advanced materials (2021) : e2008023 . |
| APA | Wang Hao , Chen Biao-Hua , Liu Di-Jia . Metal-Organic Frameworks and Metal-Organic Gels for Oxygen Electrocatalysis: Structural and Compositional Considerations. . | Advanced materials , 2021 , e2008023 . |
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摘要 ：
The shape-function relationship for designing catalysts is always a focus to study. This article describes the influence of Ni catalysts surface structure on acetone hydrogenation. We report H-2 as a morphology-directing agent to selectively synthesize branched Ni (Ni-BN), which exposes substantial stepped Ni(3 2 2) facet (similar to 99%) that has elegant activity for acetone hydrogenation. In contrary, Ni nanoparticle (Ni-NP) prepared without H-2 mainly exposes flat Ni(1 1 1) and Ni(1 0 0) facets and these facets perform less activity for acetone hydrogenation to isopropanol. Subsequently, DFT studies of reaction mechanism on different facets reveal that the step site in Ni(3 2 2) facet displays lower activation barriers than that of Ni(1 1 1) and Ni(1 0 0) facets. With help of kinetic growth model and microkinetics study, quantitative shape-function relationship of Ni-BN for acetone hydrogenation to isopropanol can be further established. This work not only clarifies the catalytic activity of Ni on acetone hydrogenation but also provides a method accessing the intrinsic kinetics of the reaction.
关键词 ：
Acetone hydrogenation Acetone hydrogenation Branched nickel Branched nickel H-2 self-select H-2 self-select High-index facet High-index facet Shape-function relationship Shape-function relationship
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| GB/T 7714 | Wang, Xiaolei , Liu, Ning , Xu, Ruinian et al. Insights into the shape effect of H-2 self-selective Ni catalysts for efficient acetone hydrogenation [J]. | APPLIED SURFACE SCIENCE , 2021 , 536 . |
| MLA | Wang, Xiaolei et al. "Insights into the shape effect of H-2 self-selective Ni catalysts for efficient acetone hydrogenation" . | APPLIED SURFACE SCIENCE 536 (2021) . |
| APA | Wang, Xiaolei , Liu, Ning , Xu, Ruinian , Chen, Biaohua , Dai, Chengna , Wu, Bin et al. Insights into the shape effect of H-2 self-selective Ni catalysts for efficient acetone hydrogenation . | APPLIED SURFACE SCIENCE , 2021 , 536 . |
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摘要 ：
1,2-Butene carbonate (BC) is an important five-membered cyclic carbonate with a high commercial value, but its massive production is limited by the lack of raw material 1,2-butanediol (1,2-BDO). 1,2-BDO is coproduced with ethylene glycol (EG) in the hydrogenation process in the coal-to-EG route, one-pot conversion of biomass to liquid fuels and chemicals, and fermentation of broths. However, the separation and purification of 1,2-BDO are difficult. In this paper, an intensified reactive distillation process for the separation of the EG and 1,2-BDO azeotropic mixture via dimethyl carbonate assisted chemical looping technology and coproduction of BC and EG products is proposed. The transesterification reactions of EG and 1,2-BDO were investigated individually in the presence of basic resin catalyst KIP321, and the kinetic parameters were imbedded into Aspen plus (V11) for the design of the reactive distillation column to perform the transesterification process. The proposed flowsheet, which includes the transesterification unit, a DMC and methanol separation unit, and an EG recovery unit, was designed and simulated. Remarkably, the conversions of diols are over 0.998, the yield of 1,2-butylene carbonate is 99.86%, and the yield of the EG product is theoretically 100%, which shows excellent potential for industrial application. © 2021 American Chemical Society
关键词 ：
Butenes Butenes Carbonation Carbonation Coal hydrogenation Coal hydrogenation Distillation Distillation Distillation columns Distillation columns Distilleries Distilleries Ethylene Ethylene Ethylene glycol Ethylene glycol Hydrogen fuels Hydrogen fuels Mixtures Mixtures Polyols Polyols Purification Purification Transesterification Transesterification
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| GB/T 7714 | Wang, Rui , Li, Hong , Gao, Xin et al. Application of dimethyl carbonate assisted chemical looping technology in the separation of the ethylene glycol and 1,2-butanediol mixture and coproduction of 1,2-butene carbonate [J]. | Industrial and Engineering Chemistry Research , 2021 , 60 (5) : 2249-2264 . |
| MLA | Wang, Rui et al. "Application of dimethyl carbonate assisted chemical looping technology in the separation of the ethylene glycol and 1,2-butanediol mixture and coproduction of 1,2-butene carbonate" . | Industrial and Engineering Chemistry Research 60 . 5 (2021) : 2249-2264 . |
| APA | Wang, Rui , Li, Hong , Gao, Xin , Wang, Yiwei , Dai, Chengna , Chen, Biaohua et al. Application of dimethyl carbonate assisted chemical looping technology in the separation of the ethylene glycol and 1,2-butanediol mixture and coproduction of 1,2-butene carbonate . | Industrial and Engineering Chemistry Research , 2021 , 60 (5) , 2249-2264 . |
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摘要 ：
Surface segregation constitutes an efficient approach to enhance the alkaline hydrogen evolution reaction (HER) activity of bimetallic PtxNiy nanoalloys. Herein, a new strategy is proposed by utilizing the small gas molecule of H2 as the structure directing agent (SDA) to in situ induce Pt surface segregations over a series of PtNi5-n samples with extremely low Pt doping (Pt/Ni = 0.2). Impressively, the sample of PtNi5-0.3 synthesized under 0.3 MPa H2 delivers an extremely low overpotential of 26.8 mV (−10 mA cm−2) and Tafel slope of 19.2 mV dec−1, which is superior to most of the previously reported PtxNiy electrocatalysts. This is substantially related to the strong H2 in situ inducing effect to generate Pt-rich@Ni-rich core-shell nanostructure of PtNi5-0.3 with an ultrahigh Pt surface content of 46%. The specific mechanistic effects of H2 during the PtNi5-n synthesis process are well illustrated based on the combined experimental and theoretical studies. The density functional theory mechanism simulations further unravel that the evolved active site of PtNi5-n can efficiently reduce the reaction Gibbs free energies; especially for the scenario of PtNi5-0.3, the downward-shifted d band center of the Pt active site significantly reduces the Pt-H bond strength, eventually resulting in the lowest absolute value of ΔGH. © 2021 Wiley-VCH GmbH
关键词 ：
Binary alloys Binary alloys Density functional theory Density functional theory Electrocatalysts Electrocatalysts Gibbs free energy Gibbs free energy Hydrogen evolution reaction Hydrogen evolution reaction Platinum Platinum Surface segregation Surface segregation
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| GB/T 7714 | Zhang, Cong , Liang, Xin , Xu, Ruinian et al. H2 In Situ Inducing Strategy on Pt Surface Segregation Over Low Pt Doped PtNi5 Nanoalloy with Superhigh Alkaline HER Activity [J]. | Advanced Functional Materials , 2021 , 31 (14) . |
| MLA | Zhang, Cong et al. "H2 In Situ Inducing Strategy on Pt Surface Segregation Over Low Pt Doped PtNi5 Nanoalloy with Superhigh Alkaline HER Activity" . | Advanced Functional Materials 31 . 14 (2021) . |
| APA | Zhang, Cong , Liang, Xin , Xu, Ruinian , Dai, Chengna , Wu, Bin , Yu, Gangqiang et al. H2 In Situ Inducing Strategy on Pt Surface Segregation Over Low Pt Doped PtNi5 Nanoalloy with Superhigh Alkaline HER Activity . | Advanced Functional Materials , 2021 , 31 (14) . |
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摘要 ：
Metal-organic frameworks (MOFs) have undergone a rapid research expansion as unpyrolyzed oxygen electrocatalysts due to their flexible and variable compositions and structures. However, the most studied MOFs possess microporous nature, which limits the mass-transfer properties and reduce the space to store insoluble discharge product of aprotic metal-air batteries. We herein report a partial ligand removal approach to create mesopore defects and unsaturated coordination in primarily microporous Cu-BTC (BTC = 1,3,5-bezenetricarboxylic acid). The mesopores were engineered by introducing isophthalic acid as a partial ligand, which has one carboxylic group missing compared to BTC, to construct mesoporous Cu-BTC (MCu-BTC). MCu-BTC was further loaded by Co species (Co/MCu-BTC) to boost the bifunctional catalytic performance toward oxygen reduction and oxygen evolution reactions. The electrochemical characterizations indicate that the mesopores of MCu-BTC enhanced the discharging capacity (ca. 7000 mAh.g(-1)) of Co-10/MCu-BTC in an aprotic Li-air battery owing to the mesopores, which allowed electrolyte infiltration for both mass and charge transfer and provided more space to store the discharge product. Further modeling simulations shed light on the contribution of the unsaturated coordination by significantly promoting the electronic conductivity and generating adequate interactions with reactants, leading to enhanced mass- and charge-transfer properties.
关键词 ：
Mesoporous metal-organic frameworks Mesoporous metal-organic frameworks metal-air battery metal-air battery oxygen evolution reaction oxygen evolution reaction oxygen reduction reaction oxygen reduction reaction unsaturated coordination unsaturated coordination
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| GB/T 7714 | Wang, Hao , Yin, Fengxiang , Liu, Ning et al. Engineering Mesopores and Unsaturated Coordination in Metal-Organic Frameworks for Enhanced Oxygen Reduction and Oxygen Evolution Activity and Li-Air Battery Capacity [J]. | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2021 , 9 (12) : 4509-4519 . |
| MLA | Wang, Hao et al. "Engineering Mesopores and Unsaturated Coordination in Metal-Organic Frameworks for Enhanced Oxygen Reduction and Oxygen Evolution Activity and Li-Air Battery Capacity" . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING 9 . 12 (2021) : 4509-4519 . |
| APA | Wang, Hao , Yin, Fengxiang , Liu, Ning , Yu, Haiyan , Fan, Tianyu , Chen, Biaohua . Engineering Mesopores and Unsaturated Coordination in Metal-Organic Frameworks for Enhanced Oxygen Reduction and Oxygen Evolution Activity and Li-Air Battery Capacity . | ACS SUSTAINABLE CHEMISTRY & ENGINEERING , 2021 , 9 (12) , 4509-4519 . |
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摘要 ：
1-Ethyl-3-methylimidazolium bis[(trifluoromethyl)sulfonyl]imide ([EMIM][Tf2N]) ionic liquid as a novel absorbent has excellent performance in BTX absorption. However, compared with the traditional method using triethylene glycol (TEG), the sustainability of the former is unknown. Thus, to bridge the gap and give a comprehensive evaluation of its industrialization potential, a methodology-integrated energetic, economic, and environmental assessment was employed. The assessment results show that the heating and cooling energy consumptions of the TEG process are 1.08 and 0.74 times higher than those of the [EMIM][Tf2N] process, respectively. But through heat integration, 5% hot and 3.4% cold utilities can be saved for the [EMIM][Tf2N] process. In terms of economic performance, the total annual costs for TEG and [EMIM][Tf2N] processes are 0.6111 and 0.4841 M$/year, respectively, and the latter is 26.3% lower than the former. As for the environmental assessment, the results indicated that compared with the TEG scenario, the [EMIM][Tf2N] scenario without absorbent recovery presented higher environmental burdens in all categories, and the largest difference lies in acidification, for which the latter is 42 times that of the former. However, when considering the absorbent recovery, the results are contradictory. Thus, the comprehensive assessment methodology proved that the [EMIM][Tf2N]-based BTX absorption process is sustainable and can be a potential industrialization technology. © 2021 American Chemical Society.
关键词 ：
Energy utilization Energy utilization Sustainable development Sustainable development Absorption Absorption Ionic liquids Ionic liquids Industrial economics Industrial economics
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| GB/T 7714 | Wu, Bin , Yu, Gangqiang , Liu, Ning et al. Deciphering the Sustainability of an Ionic Liquid-Based BTX Harvesting Process from Energetic, Environmental, and Economic Perspectives [J]. | ACS Sustainable Chemistry and Engineering , 2021 , 9 (2) : 863-873 . |
| MLA | Wu, Bin et al. "Deciphering the Sustainability of an Ionic Liquid-Based BTX Harvesting Process from Energetic, Environmental, and Economic Perspectives" . | ACS Sustainable Chemistry and Engineering 9 . 2 (2021) : 863-873 . |
| APA | Wu, Bin , Yu, Gangqiang , Liu, Ning , Xu, Ruinian , Chen, Biaohua , Dai, Chengna . Deciphering the Sustainability of an Ionic Liquid-Based BTX Harvesting Process from Energetic, Environmental, and Economic Perspectives . | ACS Sustainable Chemistry and Engineering , 2021 , 9 (2) , 863-873 . |
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