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Enhanced proton conductivity of viscose-based membranes via ionic modification and dyeing processes for fuel cell applications

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Journal of Materiomics 2023年第3期9卷 587-600页

作者： Haoyu Wu Tianchi Zhou Bin Wang Jinli Qiao Flexible Functional Materials Institute Yancheng Institute of Technology1 Hope Avenue RoadYancheng224051China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua University2999 Ren'min North RoadShanghai201620China Shanghai Engineering Research Center of Marine Renewable Energy Shanghai201306China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

Proton exchange membranes(PEMs),which are crucial fuel cell parts,play an important role in the field of energy science.However,the further development of conventional PEMs based on synthetic polymers is greatly limited by high energy consumption and difficult degradation.In this work,we reported the fabrication of a novel viscose-based PEM via cationic modification and dyeing treatment with the reactive dyes KE-7B1.High-efficiency proton transmission channels can be constructed due to the for-mation of the complex internal three-dimensional network of the as-prepared viscose-based PEM.Hþconductivity(sHþ)and water uptake are intensively investigated by changing the cationic agents and KE-7B1,and the maximum sHþreaches 44.19 mS/cm at 80℃and 98%relative humidity(RH).Furthermore,the prepared membrane shows the lowest calculated activation energy value(12.25 kJ/mol),indicating that both Grotthuss and Vehicle mechanisms play an important role in ionic transport.The membrane chemical structure and micromorphology are analyzed and the proton transmission modes are explored in detail,supplemented with research on the hydrophilic/hydrophobic characteristics and crystallinity of the membranes.The application stability of the membranes is also evaluated analyzing the thermal,mechanical,and oxygen resistance properties,and the results show that all the prepared membranes can maintain good thermal stability within 200℃.The maximum tensile strength reaches 42.12 MPa,and the mass losses of the membranes soaked in 30%(in mass,same below)H_(2)O_(2)solution for 120 h can be restricted to 10%.Therefore,as a novel PEM,the obtained dye viscose-based membranes show great potential for application in fuel cells.

关键词： Membrane Viscose Reactive dyes Proton conductivity Fuel cell

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Rational Design of Atomic Site Catalysts for Electrocatalytic Nitrogen Reduction Reaction:One Step Closer to Optimum Activity and Selectivity

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Electrochemical Energy Reviews 2022年第3期5卷 105-136页

作者： Yiran Ying Ke Fan Jinli Qiao Haitao Huang Department of Applied Physics and Research Institute for Smart Energy The Hong Kong Polytechnic UniversityHung HomKowloonHong KongChina State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua University2999 Renmin North RoadShanghai 201620China

The electrocatalytic nitrogen reduction reaction(NRR)has been one of the most intriguing catalytic reactions in recent years,providing an energy-saving and environmentally friendly alternative to the conventional Haber–Bosch process for ammonia production.However,the activity and selectivity issues originating from the activation barrier of the NRR intermediates and the competing hydrogen evolution reaction result in the unsatisfactory NH_(3) yield rate and Faradaic efficiency of current NRR catalysts.Atomic site catalysts(ASCs),an emerging group of heterogeneous catalysts with a high atomic utilization rate,selectivity,and stability,may provide a solution.This article undertakes an exploration and systematic review of a highly significant research area:the principles of designing ASCs for the NRR.Both the theoretical and experimental progress and state-of-the-art techniques in the rational design of ASCs for the NRR are summarized,and the topic is extended to double-atom catalysts and boron-based metal-free ASCs.This review provides guidelines for the rational design of ASCs for the optimum activity and selectivity for the electrocatalytic NRR.

关键词： Nitrogen reduction reaction Atomic site catalysts Design principles Activity Selectivity

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Editorial for the special issue“CO_(2)Reductions to Fuels and Carbon Feedstocks”

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Materials Reports(Energy) 2023年第2期3卷 1-3页

作者： Jinli Qiao Donghua University China

The rapid development of the industrial age is accompanied by the massive consumption of fossil energy,which leads to the massive emission of CO_(2)and triggers the global greenhouse effect.Meantime,the constant consu... 详细信息

关键词： effect. massive greenhouse

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Prediction of the geological indicators in TBM tunnel based on optimized proportion of surrounding rock grades

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Underground Space 2023年第4期11卷 204-217页

作者： Xiao Guo Wei Guo Jianqin Liu Jinli Qiao Guisong Hu School of Mechanical Engineering Tianjin UniversityTianjin 300350China Key Laboratory of Mechanism Theory and Equipment Design of Ministry of Education Tianjin UniversityTianjin 300350China School of Civil and Transportation Engineering Hebei University of TechnologyTianjin 300401China

With tunnel boring machine being used in underground engineering,accurate geological indicators have been the important basis for tunnel boring machine(TBM)construction.Back propagation neural network(BPNN)has been used to predict the geological indicators of tunnels in previous studies.Nevertheless,these studies ignored the imbalance proportion of surrounding rock grades,leading to the indiscriminate use of data,thus affecting the predictive effect of BPNN.In order to prove the importance of the proportion of surround-ing rock grade in geological prediction,we mainly attempt to utilize particle swarm optimization(PSO)to optimize the proportion of sample data,and integrate with BPNN to establish a PSO-BPNN theoretical model to predict geological indicators.At the same time,combined with the actual engineering data,5 tunneling indicators were selected as input and 4 geological indicators were selected as out-put by a variety of dimensionality reduction methods.The geological indicators are density,uniaxial compressive strength,internal fric-tion angle(u)and Poisson’s ratio(e).On this basis,the PSO-BPNN prediction model was established in detail.By comparing the prediction of traditional BPNN,PSO-BPNN and other optimization-integrated models,the result shows that optimized proportion of surrounding rock grades reduces the prediction error and improves the interpretability of the prediction model.Meanwhile,we com-bined the theory of surrounding rock partition to illustrate the rationality of surrounding rock proportion in PSO result,that is,the proportion of complex surrounding rock should be increased appropriately to improve the prediction result.Ultimately,based on the optimization-integrated models with engineering data and the surrounding rock classification theory,the importance of proportion of surrounding rock grades for tunnel geological prediction is confirmed.

关键词： TBM BPNN Particle swarm optimization Prediction of geological indicators Sample imbalance

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Atomically Dispersed Transition Metal-Nitrogen-Carbon Bifunctional Oxygen Electrocatalysts for Zinc-Air Batteries:Recent Advances and Future Perspectives

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Nano-Micro Letters 2022年第2期14卷 257-281页

作者： Fang Dong Mingjie Wu Zhangsen Chen Xianhu Liu Gaixia Zhang Jinli Qiao Shuhui Sun Institut National de La Recherche Scientifique(INRS)-CentreÉnergie Matériaux Télécommunications VarennesQC J3X 1P7Canada Key Laboratory of Materials Processing and Mold Ministry of EducationZhengzhou UniversityZhengzhou 450002People’s Republic of China State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringShanghai Innovation Institute for MaterialsDonghua UniversityShanghai 201620People’s Republic of China Engineering Research Center of Nano Geomaterials of Ministry of EducationChina University of GeosciencesWuhan 430074People’s Republic of China

Rechargeable zinc-air batteries(ZABs)are currently receiving extensive attention because of their extremely high theoretical specific energy density,low manufacturing costs,and environmental friendliness.Exploring bifunctional catalysts with high activity and stability to overcome sluggish kinetics of oxygen reduction reaction and oxygen evolution reaction is critical for the development of rechargeable ZABs.Atomically dispersed metal-nitrogen-carbon(M-N-C)catalysts possessing prominent advantages of high metal atom utilization and electrocatalytic activity are promising candidates to promote oxygen electrocatalysis.In this work,general principles for designing atomically dispersed M-N-C are reviewed.Then,strategies aiming at enhancing the bifunctional catalytic activity and stability are presented.Finally,the challenges and perspectives of M-N-C bifunctional oxygen catalysts for ZABs are outlined.It is expected that this review will provide insights into the targeted optimization of atomically dispersed M-N-C catalysts in rechargeable ZABs.

关键词： Atomically dispersed metal-nitrogen-carbon Oxygen evolution reaction(OER) Oxygen reduction reaction(ORR) Bifunctional oxygen electrocatalysts Zinc-air batteries(ZABs)

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In-situ growth of CoNi bimetal anchored on carbon nanoparticle/nanotube hybrid for boosting rechargeable Zn-air battery

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Journal of Energy Chemistry 2022年第3期31卷 348-355,I0010页

作者： Jun Li Yongxia Wang Zhengyu Yin Rui He Yihao Wang Jinli Qiao State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua UniversityShanghai 201620China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China

Exploring highly efficient non-precious metal based catalysts for bifunctional oxygen electrode is crucial for rechargeable metal-air batteries.In this study,with MOFs as precursors,a facile coprecipitation method is designed to realize in-situ growth of the CoNi anchored carbon nanoparticle/nanotube(CoNi/N-CNN)hybrid,which can achieve the simultaneous maximum exposure of both oxygen evolution reaction(OER)and oxygen reduction reaction(ORR)active centers.Benefiting from the unique structure,the CoNi/N-CNN catalyst exhibits excellent electrocatalytic performance for ORR(E_(onset)=1.183 V,E_(1/2)=0.819 V)and a low operating voltage of 1.718 V at 10 mA cm^(−2)(Ej=10)for OER.Delightfully,the home-made rechargeable Zn-air battery with CoNi/N-CNN delivers a high discharge power density up to 209 mW cm^(−2),and an outstanding charge–discharge cycling stability.The boosted bifunctional electrocatalytic activity can be ascribed to the strong coupling effect between Co/Ni center sites and defect-rich N-anchored carbon featured with porous and nanotube structure,which can introduce uniformly dispersed active sites,tailored electronic configuration,superb conductivity and convenient charge transfer process.The hybrid non-precious bimetal based electrocatalyst provides the possibility to develop the low-cost and high-efficient ORR/OER bifunctional electrocatalysts in rechargeable metal-air battery.

关键词： Co Ni/N-CNN Bifunctional electrocatalyst Oxygen electrode Rechargeable Zn-air battery

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Preparation optimization of multilayer-structured SnO_2–Sb–Ce/Ti electrode for efficient electrocatalytic oxidation of tetracycline in water

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Chinese Journal of Chemical Engineering 2018年第12期26卷 2622-2627页

作者： Kun Yang Yuyu Liu Jiawen Liu Jinli Qiao Institute of Sustainable Energy/College of Science Shanghai UniversityShanghai 200444China State Environmental Protection Engineering Center for Pollution Treatment and Control in Textile Industry College of Environmental Science and EngineeringDonghua UniversityShanghai 201620China ShanghaiJinyuan Senior High School Shanghai 200333China

In this study, electrodeposition and thermal decomposition were alternatively used for the fabrication of a series of novel multilayer-structured SnO_2–Sb–Ce/Ti(SSCT) electrodes, and their physiochemical and electrochemical properties were investigated for electrochemical oxidation of tetracycline(TC) in aqueous medium.Experimentally, after the SnO_2–Sb–Ce(SSC) composite was electrodeposited for 120 s on the titanium substrate in aqueous solution, the outer thermal coatings composed of SSC were synthesized by a hydrothermal method.Both influences of electrodeposition time(T_(ed)) and thermal decomposition time(Ttd) were investigated to obtain the optimum preparation. It was found that when increasing T_(ed)to a certain extent a longer lifetime of electrode can be achieved, which was attributed to a more solid interlayer structure. A notable SSCTT_(ed),Ttdelectrode,i.e., SSCT3,10, which was prepared through three times of 120 s' electrodeposition(T_(ed)= 3) and ten times of thermal decomposition(Ttd= 10) obtained the highest oxygen evolution potential 3.141 V vs. SCE. In this selected electrode, when 10 mg·L^(-1) initial TC concentration was added to this wastewater, the highest color removal efficiency and mineralization rate of TC were 72.4% and 41.6%, respectively, with an applied electricity density of 20 m A·cm^(-2) and treatment time of 1 h. These results presented here demonstrate that the combined application of electrodeposition and thermal decomposition is effective in realization of enhanced electrocatalytic oxidation activity.

关键词： Multilayer structured electrode Nano-hollow sphere Antibiotics Electro-oxidation

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A novel composite(FMC)to serve as a durable 3D-clam-shaped bifunctional cathode catalyst for both primary and rechargeable zinc-air batteries

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Science Bulletin 2017年第17期62卷 1216-1226页

作者： Nengneng Xu Xuemei Li Haoran Li Yanan Wei Jinli Qiao State Key Laboratory for Modification of Chemical Fibers and Polymer Materials State Environmental Protection Engineering Center for Pollution Treatment and Control inTextile IndustryCollege of Environmental Science and EngineeringDonghua UniversityShanghai 201620China

Novel and highly durable air cathode electrocatalyst with three dimensional(3D)-clam-shaped structure,MnO_2nanotubes-supported Fe_2O_3(Fe_2O_3/MnO_2) composited by carbon nanotubes(CNTs)((Fe_2O_3/MnO_2)3/4-(CNTs)_(1/4)) is synthesized using a facile hydrothermal process and a following direct heattreatment in the air. The morphology and composition of this catalyst are analyzed using scanning electronic microscopy(SEM), transmission electron microscopy(TEM), X-ray diffraction(XRD) and energy dispersive X-ray spectroscopy(EDX). The morphology characteristics reveal that flower-like Fe_2O_3 particles are highly dispersed on both MnO_2 nanotubes and CNT surfaces, coupling all three components firmly. Electrochemical measurements indicate that the synergy of catalyst exhibit superior bifunctional catalytic activity for both oxygen reduction reaction(ORR) and oxygen evolution reaction(OER) as well as stability than Pt/C and IrO_2 catalysts. Using these catalysts for air-cathodes, both primary and rechargeable zinc-air batteries(ZABs) are assembled for performance validation. In a primary ZAB,this 3D-clamed catalyst shows a decent open circuit voltage(OCV, $1.48 V) and a high discharge peak power density(349 mW cm^(-2)), corresponding to a coulombic efficiency of 92%. In a rechargeable ZABs with this bifunctional catalyst, high OCV(>1.3 V) and small charge-discharge voltage gap(<1.1 V) are achieved along with high specific capacity(780 mAh g^(-1) at 30 mA cm^(-2)) and robust cycle-life(1,390 cycles at cycle profile of 20 mA/10 min).

关键词：碳纳米管复合材料阴极催化剂双功能催化剂锌空气电池可充电三维耐用扫描电子显微镜

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Poly(vinyl alcohol)/Poly(diallyldimethylammonium chloride)anionexchange membrane modified with multiwalled carbon nanotubes for alkaline fuel cells

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Journal of Materiomics 2019年第2期5卷 286-295页

作者： Tianchi Zhou Min Wang Xuemei He Jinli Qiao YanCheng Institute of Technology 9 Ying'bing RoadYancheng224051China College of Environmental Science and Engineering Donghua University2999 Ren'min North RoadShanghai201620China Yancheng Vocational Institute of Industry Technology 285 Jiefang South RoadYancheng224005China

Hydroxyl anion conducting membrane composed of poly(vinyl alcohol)(PVA),poly(diallyldimethylammonium chloride)(PDDA),and hydroxylated multiwalled carbon nanotubes(MWCNTs-OH)have been synthesized via a facile blending-casting method assisted by a hot-chemical cross-linking process.Fourier-transform infrared spectroscopy(FTIR)and scanning electron microscopy(SEM)showed that PDDA and MWCNTs-OH were successfully introduced into the PVA matrix and MWCNTs-OH could effectively improve the network structure of the membrane.With the addition of MWCNTs-OH,many properties of the membranes such as thermal,chemical,mechanical stability and swelling property were improved significantly.Most prominent is the improvement of mechanical property,where the PVA/PDDA/MWCNTs-OH(1:0.5/3 wt.%)membrane showed high tensile strength of 40.3 MPa,tensile elongation of 12.3%and high Young's modulus of 782.8 MPa.Moreover,MWCNTs-OH bound the polymer chains in the membranes more compactly,resulting in decreased water uptake.By tuning the mass fraction of PVA,PDDA,and MWCNTs-OH in the membrane,the maximum OH-conductivity(0.030 S cm^(-1)at room temperature)was achieved for the composition of 0.5 wt.%MWCNTs-OH doped with the PVA:PDDA(1:0.5 by mass)blend.The membranes showed excellent oxidative stability when treated with both a solution of H_(2)O_(2)(30 wt.%)at room temperature and in a hot KOH solution(8 M)at 80℃.Based on the full aliphatic structure membrane(PVA/PDDA-OH/1 wt.%MWCNTs-OH),membrane electrode assemblies(MEAs)fabricated with Pt/C cathode catalyst can achieve power densities of 41.3 mW cm^(-2)and 66.4 mW cm^(-2)in a H_(2)/O_(2)system at room temperature and 40℃,respectively.Using CoPc as the Pt-free cathode catalyst,power densities of 9.1 mW cm^(-2)and 14.0 mW cm^(-2)at room temperature and 40℃ were obtained,respectively.

关键词： Alkaline membrane Conductivity CNT doping Stability Fuel cell

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Imidazolium group prompted alkaline anion-exchange membrane with high performance for efficient electrochemical CO_(2) conversion

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Green Energy & Environment 2023年第3期8卷 893-903页

作者： Min Wang Qianqian Zou Xueqi Dong Nengneng Xu Rong Shao Jianfei Ding Yidong Zhang Jinli Qiao School of Chemistry and Chemical Engineering Yancheng Institute of TechnologyYancheng224051China Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092College of Environmental Science and EngineeringDonghua University2999 Ren'min North RoadShanghai201620China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China

Development of high-performance hydroxide-conductive membranes is a focus research subject owing to promising applications in electrochemical reduction of CO_(2)(eCO_(2)RR).However,few satisfactory membranes have been developed to maximize the performance of CO_(2) electrolyzers,despite its role as the core in regulating ion transport and preventing product crossover or fuel loss.Herein,we report the synthesis of alkaline anion-exchange membranes fabricated by poly(vinyl-alcohol)(PVA)and poly[(3-methyl-1-vinylimidazoliummethylsulfate)-co-(1-vinylpyrrolidone)](PQ44)for use in CO_(2) electrolysis.Owing to the unique imidazolium ring structure coupled with a three-dimensional semiinterpenetrating porous internal architecture,the PVA/PQ44-OH-membranes provide a high hydroxide conductivity(21.47 mS cm^(-1)),preferable mechanical property and thermal stability.In particular,the eCO_(2)RR used PVA/PQ44-OH^(-) as electrolyte membrane realized a charming Faradaic efficiency(88%)and partial current density(29 mA cm^(-2))at0.96 VRHE and,delivered the excellent durability over 20 h electrolysis in 0.5 mol L^(-1) KHCO_(3) electrolyte.Notably,it can even enable an ultrahigh current density beyond 100 mA cm^(-2) at^(-1).11 VRHE when the electrolyte was KOH instead,and produced the FEHCOOof 85%at a low potential of0.81 VRHE,superior to both commercial alkaline A201 and acidic Nafion117 membrane.

关键词： Alkaline anion-exchange membrane Imidazolium ring structure Semi-interpenetrating network CO_(2)electroreduction Formate production

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