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Ionic liquids for CO_(2) electrochemical reduction

Chinese Journal of Chemical Engineering 2021年第3期34卷 75-93页

作者： Fangfang Li Francesca Mocci Xiangping Zhang Xiaoyan Ji Aatto Laaksonen Energy Engineering Division of Energy ScienceLuleåUniversity of TechnologyLuleå97187Sweden Department of Chemical and Geological Sciences University of CagliariMonserrato 09042Italy CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China Division of Physical Chemistry Department of Materials and Environmental ChemistryArrhenius LaboratoryStockholm UniversityStockholm 10691Sweden Center of Advanced Research in Bionanocojugates and Biopolymers “Petru Poni”Institute of Macromolecular ChemistryIasi 700469Romania State Key Laboratory of Materials-Oriented and Chemical Engineering Nanjing Tech UniversityNanjing 211816China

Electrochemical reduction of CO_(2) is a novel research field towards a CO_(2)-neutral global economy and combating fast accelerating and disastrous climate changes while finding new solutions to store renewable energy in value-added chemicals and *** liquids(ILs),as medium and catalysts(or supporting part of catalysts)have been given wide attention in the electrochemical CO_(2) reduction reaction(CO_(2) RR)due to their unique advantages in lowering overpotential and improving the product selectivity,as well as their designable and tunable *** this review,we have summarized the recent progress of CO_(2) electro-reduction in IL-based electrolytes to produce higher-value *** then have highlighted the unique enhancing effect of ILs on CO_(2) RR as templates,precursors,and surface functional moieties of electrocatalytic ***,computational chemistry tools utilized to understand how the ILs facilitate the CO_(2) RR or to propose the reaction mechanisms,generated intermediates and products have been discussed.

关键词： Carbon dioxide Ionic liquids Electro-reduction Electrolyte Electrocatalytic material Computer simulation

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Numerical simulation of coal gasifier for hydrogen product and in-situ fixation of CO2

Numerical simulation of coal gasifier for hydrogen product a...

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2007 AIChE Annual Meeting

作者： Lu, Jing Yu, Liang Zhang, Xiangping Zhang, Suojiang Dai, Wenbin State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences Beijing 100080 China China Graduate University Chinese Academy of Sciences 100049 Beijing China Advanced Systems Center Mitsubishi Materials Corporation Tokyo 112-0002 Japan

ISBN: (纸本)9780816910229

In order to eliminate the global warming effect, it is highly required to develop new technologies with lower or zero emission of CO2 to the environment. In this work, a fluidized bed coal gasifier with in-situ fixation of CO2 is simulated by developing a comprehensive two-dimensional unsteady state model. Eddy Dissipation Concept (EDC) model is adopted for describing the turbulent mixing and detailed chemical kinetics simultaneously. The profiles of temperature, velocity and reaction rate, and particle trajectories are predicted and analyzed, also the mechanism of flow and reaction, including the in-situ fixation process of CO2, is discussed. Comparing with the traditional coal gasifier without CaO, a much higher concentration of H2 (traditional: 5.78 vol%, present: 65.43 vol%) and lower concentration of CO (traditional: 37.15 vol%, present: 10.51 vol%) and CO2 (traditional: >45 vol%, present: 14.05 vol%) are obtained.

关键词： Carbon dioxide

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Ultrathin curved PdNiRu nanosheets as bifunctional catalysts for oxygen reduction and ethylene glycol oxidation

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Nano Research 2024年第5期17卷 3777-3784页

作者： Xianzeng Li Tingyu Lu Huan Pang Mingyi Zhang Dongdong Xu Lin Xu Min Han Jun Yang Jiangsu Key Laboratory of New Power Batteries Jiangsu Collaborative Innovation Center of Biomedical Functional MaterialsSchool of Chemistry and Materials ScienceNanjing Normal UniversityNanjing 210023China Fujian Cross Strait Institute of Flexible Electronics(Future Technology) Fujian Normal UniversityFuzhou 350117China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China State Key Laboratory of Coordination Chemistry Nanjing UniversityNanjing 210023China School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhou 225009China Key Laboratory for Photonic and Electronic Bandgap Materials Ministry of EducationSchool of Physics and Electronic EngineeringHarbin Normal UniversityHarbin 150025China

Pd-based metallic nanosheets with advanced physicochemical properties have been widely prepared and employed in various electrocatalytic ***,few concerns were focused on their multiple performances in different ***,highly curved and ultrathin PdNiRu nanosheets(NSs)are developed by facile wet-chemistry strategy and exhibit excellent electrocatalytic performance toward both oxygen reduction reaction(ORR)and ethylene glycol oxidation reaction(EGOR).Owing to the synergistically structural(e.g.,ultrathin,curved,defects/steps-rich)and compositional(ternary alloy)advantages,PdNiRu NSs exhibited enhanced ORR and EGOR specific/mass activities and better stability/durability than control *** specific activity(5.52 mA·cm^(−2))and mass activity(1.13 A·mg_(Pd)^(−1))of the PdNiRu NSs in ORR are 4.8 and 3.4 times as the ones of commercial Pt/C,*** mass activity of PdNiRu NSs(3.86 A·mg_(Pd)^(−1))in EGOR is 2.6 times as commercial Pd/C(1.51 A·mg_(Pd)^(−1)).This study is helpful for the development of desired electrocatalysts with multi-functional application in practical fuel cells.

关键词： ultrathin nanosheets noble metal electrocatalysts bifunctional

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A perspective of chalcogenide semiconductor-noble metal nanocomposites through structural transformations

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Nano Materials Science 2019年第3期1卷 184-197页

作者： Danye Liu Linlin Xu Jianping Xie Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences No.19A Yuquan RoadBeijing100049China Department of Chemical and Biomolecular Engineering National University of Singapore4 Engineering Drive 4117585Singapore Center for Mesoscience Institute of Process EngineeringChinese Academy of SciencesBeijing100190China Zhongke Langfang Institute of Process Engineering Fenghua Road No 1Langfang Economic&Technical Development ZoneHebei Province065001China

Intense efforts have been devoted to the synthesis of heterogeneous nanocomposites consisting of chalcogenide semiconductors and noble metals,which usually exhibit enhanced properties owing to the synergistic effect between their different material *** the structure of the metal domains in the nanocomposites may lead to further improvements of its performance for a given *** review therefore highlights the strategies based on a structural conversion process for the fabrication of nanocomposites consisting of chalcogenide semiconductors and noble metals with various internal structures,e.g.,hollow or *** strategy relies on a unique inside-out diffusion phenomenon of Ag in core-shell nanoparticles with Ag residing at core or inner shell *** the presence of sulfur or selenium precursors,the diffused Ag are converted into Ag2S or Ag2Se,which is connected with the remaining noble metal parts,forming nanocomposites consisting of silver chalcogenide and noble metal nanoparticles with hollow or cage-bell *** would focus on the introduction of the fundamentals,principles,electrocatalytic applications as well as perspectives of the chalcogenide semiconductor-noble metal nanocomposites derived from their core-shell precursors so as to provide the readers insights in designing efficient nanocomposites for electrocatalysis.

关键词： Nanocomposite Chalcogenide Noble metal Nanoparticle Structural conversion Electrocatalysis

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Reactive template-derived interfacial engineering of CoP/CoO heterostructured porous nanotubes towards superior electrocatalytic hydrogen evolution

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Carbon Energy 2023年第1期5卷 194-205页

作者： Qixing Zhou Ruoxu Sun Yiping Ren Run Tian Jun Yang Huan Pang Kai Huang Xinlong Tian Lin Xu Yawen Tang School of Chemistry and Chemical Engineering Southeast UniversityNanjingJiangsuChina State Key Laboratory of Marine Resource Utilization in South China Sea Hainan Provincial Key Lab of Fine ChemistrySchool of Chemical Engineering and TechnologyHainan UniversityHaikouHainanChina Jiangsu Key Laboratory of New Power Batteries School of Chemistry and Materials ScienceJiangsu Collaborative Innovation Center of Biomedical Functional MaterialsNanjing Normal UniversityNanjingJiangsuChina Nanjing IPE Institute of Green Manufacturing Industry NanjingJiangsuChina State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijingChina School of Chemistry and Chemical Engineering Yangzhou UniversityYangzhouJiangsuChina

The development of economical,efficient,and robust electrocatalysts toward the hydrogen evolution reaction(HER)is highly imperative for the rapid advancement of renewable H2 energy-associated *** utilization of the heterointerface effect can endow the catalysts with remarkably boosted electrocatalytic performance due to the modified electronic state of active ***,we demonstrate deliberate crafting of CoP/CoO heterojunction porous nanotubes(abbreviated as CoP/CoO PNTs hereafter)using a self-sacrificial template-engaged *** control over the Kirkendall diffusion process of the presynthesized cobalt–aspartic acid complex nanowires is indispensable for the formation of CoP/CoO *** topochemical transformation strategy of the reactive templates enables uniform and maximized construction of CoP/CoO heterojunctions throughout all the porous *** establishment of CoP/CoO heterojunctions could considerably modify the electronic configuration of the active sites and also improve the electric conductivity,which endows the resultant CoP/CoO PNTs with enhanced intrinsic ***,the hollow and porous nanotube architectures allow sufficient accessibility of exterior/interior surfaces and molecular permeability,drastically promoting the reaction ***,when used as HER electrocatalysts,the well-designed CoP/CoO PNTs show Pt-like activity,with an overpotential of only 61 mV at 10mA cm^(−2) and excellent stability in 1.0M KOH medium,exceeding those of the vast majority of the previously reported nonprecious *** functional theory calculations further substantiate that the construction of CoP/CoO heterojunctions enables optimization of the Gibbs free energies for water adsorption and H adsorption,resulting in boosted HER intrinsic *** present study may provide in-depth insights into the fundamental mechanisms of heterojunction-induced electronic regulation,which may p

关键词： heterojunction hydrogen evolution reaction porous nanotubes reactive template

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Estimating Hansen solubility parameters of organic pigments by group contribution methods

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Chinese Journal of Chemical Engineering 2021年第3期34卷 186-197页

作者： Markus Enekvist Xiaodong Liang Xiangping Zhang Kim Dam-Johansen Georgios MKontogeorgis Center for Energy Resources Engineering(CERE) Department of Chemical and Biochemical EngineeringTechnical University of DenmarkBuilding 229Søltofts Plads 229DK-2800 Kgs.LyngbyDenmark Hempel Foundation Coatings Science and Technology Centre(CoaST) Department of Chemical and Biochemical EngineeringTechnical University of DenmarkBuilding 229Søltofts Plads 229DK-2800 Kgs.LyngbyDenmark Sino-Danish Center for Education and Research(SDC) IPEUniversity of Chinese Academy of SciencesBeijing 100049China Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China

The Hansen solubility parameters(HSP)are frequently used for solvent selection and characterization of polymers,and are directly related to the suspension behavior of pigments in solvent *** performance of currently available group contribution(GC)methods for HSP were evaluated and found to be insufficient for computer-aided product design(CAPD)of paints and coatings.A revised and,for this purpose,improved GC method is presented for estimating HSP of organic compounds,intended for organic *** to the significant limitations of GC methods,an uncertainty analysis and parameter confidence intervals are provided in order to better quantify the estimation accuracy of the proposed *** to other applicable GC methods,the prediction error is reduced significantly with average absolute errors of 0.45 MPa^(1/2),1.35 MPa^(1/2),and 1.09 MPa^(1/2) for the partial dispersion(δD),polar(δP)and hydrogen-bonding(δH)solubility parameters respectively for a database of 1106 *** performance for organic pigments is comparable to the overall method performance,with higher average errors forδD and lower average errors forδP andδH.

关键词： Hansen solubility parameters Group contribution method Organic pigments Computer-aided product design Parameter estimation Uncertainty analysis

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Molecular Architecture of Cobalt Porphyrin Multilayers on Reduced Graphene Oxide Sheets for High Performance Oxygen Reduction Reaction

Molecular Architecture of Cobalt Porphyrin Multilayers on Re...

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International Conference on Nanoscience & Technology,China 2013(ChinaNANO 2013)

作者： Hongjie Tang Huajie Yin Jiangyan Wang Nailiang Yang Dan Wang Zhiyong Tang State Key Laboratory of Multiphase Complex Systems Institute of Process Engineering Chinese Academy of Sciences National Center for Nanoscience and Technology China

Development of non-precious-metal electrocatalysts is believed as the key for realization of scale-up applications of the proton exchange membrane fuel cells. One of the most promising types of non-precious-metal catalysts is carbon-supported transition metal-nitrogen (C/M-N x ) materials (M = Co, Fe, Ni, Mn, etc., and normally x = 2 or 4). In this article, a novel molecular design strategy, in which the multilayers of Co 2+ ions and porphyrin are fabricated onto the surface of the reduced graphene oxide sheets by the layer-by-layer assembly technique, is suggested for production of the cost-effective and high-efficient catalysts. Impressively, compared with commercial carbon-supported Pt catalysts, the prepared multilayers on the surface of the reduced graphene oxide sheets exhibit the comparable electrocatalytic activity, but much better methanol tolerance and long-term stability toward oxygen reduction reaction. This work opens a door toward accurate construction of the low-cost catalysts for high-performance oxygen reduction reaction.

关键词： cobalt porphyrin, multilayers, layer-by-layer, oxygen reduction reaction

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Light doping of tungsten into copper-platinum nanoalloys for boosting their electrocatalytic performance in methanol oxidation

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Nano Research Energy 2022年第2期1卷 194-200页

作者： Danye Liu Qing Zeng Chaoquan Hu Dong Chen Hui Liu Yongsheng Han Lin Xu Qingbo Zhang Jun Yang State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Center of Materials Science and Optoelectronics Engineering University of Chinese Academy of SciencesBeijing 100049China Nanjing IPE Institute of Green Manufacturing Industry Nanjing 211100China School of Chemistry and Materials Science Jiangsu Key Laboratory of New Power BatteriesJiangsu Collaborative Innovation Centre of Biomedical Functional MaterialsNanjing Normal UniversityNanjing 210023China Department of Bioengineering Rice UniversityHoustonTexas 77005USA

Coupling the bi-functional mechanism with compressive lattice strain might be an effective way to boost the electrocatalysis of platinum(Pt)-based nanoparticles for methanol oxidation reaction(MOR).This strategy weakens the chemisorption of poisoning CO-like intermediates generated during MOR on the active Pt sites by lowering their d-band *** this context,we herein report the synthesis of ternary copper-tungsten-platinum(CuWPt)nanoalloys with light doping of W element by simply co-reducing their precursors at elevated *** this ternary alloy system,the presence of only small amount of W element not only weakens the chemisorption of CO-like intermediates by lowering the Pt d-band center through compressive lattice strain,but also cleans the active Pt sites by“hydrogen spillover effect”,endowing the as-prepared CuWPt nanoalloys at an appropriate Cu/W/Pt ratio with good activity for *** specific,the ternary CuWPt alloy nanoparticles at a Cu/W/Pt molar ratio of 21/4/75 show a specific activity of 2.5 mA·cm^(−2)and a mass activity of 2.11 A·mg^(−1)with a better durability,outperforming those ternary CuWPt alloy nanoparticles at other Cu/W/Pt ratios,binary CuPt alloys and commercial Pt/C catalyst as well as a large number of reported Pt-based *** addition,a single direct methanol fuel cell(DMFC)assembled using ternary CuWPt nanoalloys as anodic catalysts shows a power density of 24.3 mW·cm^(−2)and an open-circle voltage of 0.6 V,also much higher than those of the single DMFC assembled from commercial Pt/C catalysts.

关键词： lattice strain d-band center electrocatalysis hydrogen spillover methanol oxidation reaction

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A Web-like Three-dimensional Binder for Silicon Anode in Lithium-ion Batteries

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Energy & Environmental Materials 2024年第1期7卷 21-27页

作者： Liyuan Li Tao Li Yifan Sha Baozeng Ren Lan Zhang Suojiang Zhang CAS Key Laboratory of Green Process and Engineering Beijing Key Laboratory of Ionic Liquids Clean ProcessState Key Laboratory of Multiphase Complex SystemsInstitute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Langfang Green Industrial Technology Center Langfang 065001China Henan Key Laboratory of Energy Storage Materials and Processes Zhengzhou Institute of Emerging Industrial TechnologyZhengzhou 450003China

Si anode is of paramount importance for advanced energy-dense lithium-ion batteries(LIBs).However,the large volume change as well as stress generates during its lithiation-delithiation process poses a great challenge to the long-term cycling and hindering its *** this work,a composite binder is prepared with a soft component,guar gum(GG),and a rigid linear polymer,anionic polyacrylamide(APAM).Rich hydroxy,carboxyl,and amide groups on the polymer chains not only enable intermolecular crosslinking to form a web-like binder,A2G1,but also realize strong chemical binding as well as physical encapsulating to Si *** resultant electrode shows limited thickness change of merely 9%on lithiation and almost recovers its original thickness on *** demonstrates high reversible capacity of 2104.3 mAh g^(-1)after 100 cycles at a current density of 1800 mA g^(-1),and in constant capacity(1000 mAh g^(-1))test,it also shows a long life of 392 ***,this soft-hard combining web-like binder illustrates its great potential in the future applications.

关键词： anionic polyacrylamide lithium-ion batteries Si anode thickness change web-like binder

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Oxygen-doped carbon host with enhanced bonding and electron attraction abilities for efficient and stable SnO_2/carbon composite battery anode

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Science China Materials 2018年第8期61卷 1067-1077页

作者： Zhen Geng Bing Li Hezhi Liu Hong Lv Qiangfeng Xiao Yongjun Ji Cunman Zhang Clean Energy Automotive Engineering Center Tongji UniversityShanghai 201804China Beijing National Laboratory for Condensed Matter Physics Institute of PhysicsChinese Academy of SciencesBeijing 100190China State Key Laboratory of Multiphase Complex Systems Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China General Motors Research and Development Center WarrenMI 48090USA

The coupling between electrochemically active material and conductive matrix is vitally important for high efficiency lithium ion batteries （LIBs）. By introducing oxygen groups into the nanoporous carbon framework, we accom- plish sustainably enhanced electrochemical performance for a SnO2/carbon LIB. 2-5 nm SnO2 nanoparticles are hydro- thermally grown in different nanoporous carbon frameworks, which are pristine, nitrogen- or oxygen-doped carbons. Compared with pristine and nitrogen-doped carbon hosts, the SnO2/oxygen-doped activated carbon （OAC） composite ex- hibits a higher discharge capacity of 1,122mAhg^-1 at 500 mA g^-1 after 320 cycles operation and a larger lithium storage capacity up to 680 mAhg-I at a high rate of 2,000 mA g^-1. The exceptional electrochemical performance originated from the oxygen groups, which could act as Lewis acid sites to attract electrons effectively from Sn during the charge process, thus accelerating reversible conversion of Sn to SnO2. Meanwhile, SnO2 nanoparticles are effectively bonded with carbon through such oxygen groups, thus preventing the electrochemical sintering and maintaining the cycling stability of the SnO2/OAC composite anode. The high electrochemical performance, low biomass cost, and facile preparation renders the SnO2/OAC composites a promising candidate for anode materials.

关键词： tin oxide nanoporous carbon functional groups anode materials lithium-ion batteries

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