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Electrolyte dependence for the electrochemical decarboxylation of medium-chain fatty acids (n-octanoic acid) into fuel on Pt electrode

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Materials Reports(Energy) 2024年第2期4卷 64-70页

作者： Zhenmin Zhang Dezhang Ren Dian Zhang Tiantian Hu Congyuan Zeng nengneng xu Zhibao Huo Jinli Qiao College of Marine Ecology and Environment Shanghai Ocean UniversityShanghai201306PR China Department of Mechanical Engineering Southern University and A&M CollegeBaton RougeLA70807USA State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua UniversityShanghai201620PR China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092PR China

The deoxygenation of organic acids, important biomass feedstocks and derivatives, to synthesize hydrocarbon products under mild electrochemical conditions, holds significant importance for the production of carbon-neutral biofuels. There is still limited research on the influential factors of the electrochemical decarboxylation reaction of medium-chain fatty acids. In this study, n-octanoic acid (OA) was chosen as the research subject to investigate the electrochemical decarboxylation behavior of OA on a platinum electrode, focusing on the influence of different alkali metal cations (Li^(+), Na^(+), K^(+)), common anions (SO^(4)^(2−), Cl^(−)), and electrolyte pH. It was found that KOH as an electrolyte exhibited the best performance for OA. Possibly, the larger size of K^(+) increased the alkalinity of the electrode surface, facilitating OA deprotonation. LiOH electrolyte reduced the solubility of OA, thereby inhibiting the decarboxylation reaction. SO^(4)^(2−) exhibited a weak promoting effect on the decarboxylation reaction of OA, while Cl^(−) showed no adverse effect although Cl^(−) may adsorb on the electrode surface. Furthermore, unlike short-chain fatty acids, medium-chain OA can only achieve efficient decarboxylation under alkaline conditions due to its solubility properties. This study provides references and foundations for future efforts to enhance the efficiency of electrochemical decarboxylation synthesis of hydrocarbon biofuels from medium-chain fatty acids.

关键词： Fatty acids Kolbe reaction Decarboxylation Hydrocarbon Electrolyte

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可逆锌-空气电池锌阳极研究进展及挑战

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材料导报 2024年第6期38卷 26-35页

作者：王越周本基徐能能乔锦丽东华大学环境科学与工程学院纤维材料改性国家重点实验室上海201600

锌-空气电池因安全性高、容量大、成本低和环境友好等特点而受到广泛关注。其中,锌-空气电池阴极双功能催化剂的设计开发取得了突破性进展。因此,锌阳极的可逆性成为决定锌-空气电池充放电性能的关键。然而,锌阳极仍面临枝晶、形变、钝... 详细信息

锌-空气电池因安全性高、容量大、成本低和环境友好等特点而受到广泛关注。其中,锌-空气电池阴极双功能催化剂的设计开发取得了突破性进展。因此,锌阳极的可逆性成为决定锌-空气电池充放电性能的关键。然而,锌阳极仍面临枝晶、形变、钝化、析氢腐蚀等严重挑战,直接阻碍了可逆锌-空气电池的实际应用。为此,本文从枝晶形成、电极形变、钝化、析氢腐蚀四个方面系统介绍了锌阳极研究现状;讨论了添加剂、涂层、隔膜和充电方式对锌枝晶生长的影响;提出了电极形变的机理和常见解决方案;归纳了锌阳极发生钝化的关键因素和影响机制;分析了合金组分对析氢腐蚀的抑制。最后,基于锌阳极当前的主要研究现状,本文展望了获得稳定可逆锌阳极的多种策略及研究方向。

关键词：可逆锌空气电池锌阳极枝晶生长形变钝化析氢腐蚀

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聚乙烯醇基凝胶电解质的制备及在储能器件中的应用

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材料导报 2024年第8期38卷 57-67页

作者：钮政罗希徐能能陈刚乔锦丽东华大学环境科学与工程学院上海201600

由于在电化学能源存贮与转化器件中所展现出的巨大潜在应用前景,固态聚合物电解质膜的开发受到研究界的广泛关注。基于柔性储能与转换器件的发展,以聚乙烯醇(Polyvinyl alcohol, PVA)为基体的凝胶聚合物电解质(Gel polymer electrolytes... 详细信息

由于在电化学能源存贮与转化器件中所展现出的巨大潜在应用前景,固态聚合物电解质膜的开发受到研究界的广泛关注。基于柔性储能与转换器件的发展,以聚乙烯醇(Polyvinyl alcohol, PVA)为基体的凝胶聚合物电解质(Gel polymer electrolytes, GPEs)因亲水性强,无毒,良好的兼容性以及优异的化学稳定性,是当前研究较多的理想电解质材料。本文从PVA基水凝胶电解质的制备合成原理、方法和性能表征出发,总结和讨论了其基本物理特性和电化学性能,并就PVA基水凝胶电解质在超级电容器、柔性锌空电池、锂离子电池以及太阳能水热电池中的研究和应用进展进行了综述,并对其在该领域未来的发展做出展望。

关键词：聚乙烯醇凝胶聚合物电解质交联方式柔性储能转化器件

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锌阳极氮掺杂多孔碳表面功能层设计及可逆性研究

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材料导报 2024年第6期38卷 49-54页

作者：陈京健徐能能芦拓魏群山东华大学环境科学与工程学院上海201600

锌阳极因枝晶生长、析氢、形变和钝化等挑战,成为限制锌空气电池充放电循环性能的关键因素。本工作以聚季铵盐为碳源和氮源,通过硬模板法制备出具有丰富介孔结构的碳材料,并将其作为锌阳极的表面功能层(N-MC@Zn)。其中,N-MC@Zn的比表面... 详细信息

锌阳极因枝晶生长、析氢、形变和钝化等挑战,成为限制锌空气电池充放电循环性能的关键因素。本工作以聚季铵盐为碳源和氮源,通过硬模板法制备出具有丰富介孔结构的碳材料,并将其作为锌阳极的表面功能层(N-MC@Zn)。其中,N-MC@Zn的比表面积高达590.06 m^(2)·g^(-1),平均孔径为22 nm。研究表明,锌阳极表面构建氮掺杂的多孔碳功能层,在一定程度上有效缓解了上述寄生反应带来的负面影响。特别是多孔碳涂层丰富的孔隙为锌沉积/剥离提供了缓冲区,极大提高了锌离子的沉积动力学,稳定了其沉积/剥离过程,缓解了锌阳极的析氢腐蚀;此外,多孔碳涂层内的各向异性避免了尖端效应,抑制了枝晶生长。基于上述优势,N-MC@Zn表现出优异的充放电稳定性(140 h, 700次循环)、倍率充放电特性(0.5C~10C)以及放电容量。以上结果表明,多孔碳材料可作为高性能锌阳极功能层材料,为锌阳极涂层设计领域提供了新的视角。

关键词：锌阳极介孔碳表面改性锌枝晶锌空气电池

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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, MnO2 nanotubes-supported Fe2O3 （Fe2O3/MnO2） composited by carbon nanotubes （CNTs）（（Fe2O3/ MnO2）3/4-（CNTs）1/4） is synthesized using a facile hydrothermal process and a following direct heat- treatment in the air. The morphology and composition of this catalyst are analyzed using scanning elec- tronic microscopy （SEM）, transmission electron microscopy （TEM）, X-ray diffraction （XRD） and energy dispersive X-ray spectroscopy （EDX）. The morphology characteristics reveal that flower-like Fe2O3 parti- cles are highly dispersed on both MnO2 nanotubes and CNT surfaces, coupling all three components firmly. Electrochemical measurements indicate that the synergy of catalyst exhibit superior bi- functional catalytic activity for both oxygen reduction reaction （ORR） and oxygen evolution reaction （OER） as well as stability than Pt/C and lrO2 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 coulomhic efficiency of 92%. In a rechargeahle 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： Bifunctional composite catalysts ORR and OER Rechargeable ZABs Specific capacity Long durability

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3D hollow sphere Co_3O_4/MnO_2-CNTs:Its high-performance bi-functional cathode catalysis and application in rechargeable zinc-air battery

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Green Energy & Environment 2017年第3期2卷 316-328页

作者： xuemei Li nengneng xu Haoran Li Min Wang Lei Zhang Jinli Qiao College of Environmental Science and Engineering Donghua Universty Energy Mining & Environment National Research Council of Canada

There has been a continuous need for high active, excellently durable and low-cost electrocatalysts for rechargeable zinc-air batteries. Among many low-cost metal based candidates, transition metal oxides with the CNTs composite have gained increasing attention. In this paper, the 3-D hollow sphere MnO_2 nanotube-supported Co_3O_4 nanoparticles and its carbon nanotubes hybrid material(Co_3 O_4/MnO_2-CNTs) have been synthesized via a simple co-precipitation method combined with post-heat treatment. The morphology and composition of the catalysts are thoroughly analyzed through SEM, TEM, TEM-mapping, XRD, EDX and XPS. In comparison with the commercial 20% Pt/C, Co_3O_4/MnO_2,bare MnO_2 nanotubes and CNTs, the hybrid Co_3O_4/MnO_2-CNTs-350 exhibits perfect bi-functional catalytic activity toward oxygen reduction reaction and oxygen evolution reaction under alkaline condition(0.1 M KOH). Therefore, high cell performances are achieved which result in an appropriate open circuit voltage(～1.47 V),a high discharge peak power density(340 mW cm^(-2)) and a large specific capacity(775 mAh g^(-1) at 10 mA cm^(-2)) for the primary Zn-air battery, a small charge-discharge voltage gap and a high cycle-life(504 cycles at 10 mA cm^(-2) with 10 min per cycle) for the rechargeable Zn-air battery. In particular, the simple synthesis method is suitable for a large-scale production of this bifunctional material due to a green, cost effective and readily available process.

关键词： Bi-functional catalyst Oxygen reduction reaction Oxygen evolution reaction Activity and stability Rechargeable zinc-air battery

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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 ***,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) *** 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 *** 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) ***,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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Anion-regulation engineering toward Cu/In/MOF bimetallic electrocatalysts for selective electrochemical reduction of CO_(2) to CO/formate

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Materials Reports(Energy) 2022年第3期2卷 65-70页

作者： Bingqing xu Israr Masood Ul Hasan Luwei Peng Junyu Liu nengneng xu Mengyang Fan Nabeel Khan Niazi Jinli Qiao State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua UniversityShanghai201620China Shanghai Institute of Pollution Control and Ecological Security Shanghai200092China Institute of Soil and Environmental Sciences University of Agriculture FaisalabadFaisalabad38040Pakistan Department of Mechanical and Industrial Engineering University of TorontoTorontoOntarioM5S 3G8Canada

The conversion of carbon dioxide(CO_(2))into high-value added energy fuels and chemicals(CO,formate,C_(2)H_(4),etc.)through electrochemical reduction(eCO_(2)R)is a promising avenue to sustainable ***,low selectivity,barren activity and poor stability of the electrodes hinder the large-scale application of eCO_(2)***,we reported a copper-indium-organic-framework(CuIn-MOF)based high-performance catalyst for eCO_(2)***-trochemical measurement results reveal that CuIn-MOF exhibits high Faradaic efficiency(FE)of CO and formate(300 mV,FE_(CO)=78.6%at-0.86 V ***,FE_(HCOO^(-))=48.4%at-1.16 V ***,respectively)in a broad range of current density(20.1–88.4 mA cm^(-2))with long-term stability(6 h)for eCO_(2)R in 0.5 M KHCO_(3)electrolyte ***,through anion-regulation engineering,SO_(4)^(2-)anion precursor is more beneficial for the formic acid generation than NO_(3)^(-)anion precursor;while for SO_(4)^(2-)anion precursor,Cu plays a positive regulating role in eCO_(2)R to CO compared to ***,the high performance in a home-made eCO_(2)R reactor derives benefit from enhanced intrinsic activity and charge re-distribution can be attributed to the formation of In-doped Cu layer.

关键词： CuIn-MOF based Catalyst Anion-regulation engineering CO_(2)electroreduction CO/Formate production CO_(2)electrolyzer

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Crystal facet engineering coexposed CuIn(200)and In(101)in CuIn alloy nanocatalysts enabling selective and stable CO_(2)electroreduction

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Journal of Energy Chemistry 2023年第11期86卷 569-578,I0012页

作者： Lulu Li Yang Zhang Xi Luo Israr Masood ul Hasan Kai Wu Bing Nan Yanxing Zhang nengneng xu Jinli Qiao State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringShanghai 201620China College of Materials and Textile Engineering Jiaxing UniversityJiaxing 314001ZhejiangChina Shanghai Institute of Pollution Control and Ecological Security Shanghai 200092China Shanghai Synchrotron Radiation Facility Shanghai Advanced Research InstituteChinese Academy of SciencesShanghai 201204China School of Physics Henan Normal UniversityXinxiang 453007HenanChina Institute of Soil and Environmental Sciences University of Agriculture FaisalabadFaisalabad 38040Pakistan

The electrocatalytic carbon dioxide reduction reaction(eCO_(2)RR)into high-value-added chemicals and fuels is a promising strategy to mitigate global ***,it remains a significant stumbling block to the rationally tuning lattice plane of the catalyst with high activity to produce the target product in the eCO_(2)RR *** attempt to solve this problem,the Culn bimetallic alloy nanocatalyst with specifically exposed lattice planes is modulated and electrodeposited on the nitrogen-doped porous carbon cloth by a simple two-step electrodeposition method,which induces high Faraday efficiency of 80%towards HCOO-(FEHCOO-)with a partial current density of 13.84 mA cm-2at-1.05 V(***).Systematic characterizations and theoretical modeling reveal that the specific coexposed Culn(200)and In(101)lattice facets selectively adsorbed the key intermediate of OCHO*,reducing the overpotential of HCOOH and boosting the FEHCOO-in a wide potential window(-0.65--1.25 V).Moreover,a homogeneous distribution of Culn nanoparticles with an average diameter of merely~3.19 nm affords exposure to abundant active sites,meanwhile prohibiting detachment and agglomeration of nanoparticles during eCO_(2)RR for enhanced stability attributing to the self-assembly electrode *** study highlights the synergistic effect between catalytic activity and facet effect,which opens a new route in surface engineering to tune their electrocatalytic performance.

关键词： Electrocatalytic CO_(2) reduction reaction Culn alloy Crystal facetengineering Nanocatalyst

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Carbon‐based metal‐free catalysts for electrochemical CO2 reduction: Activity, selectivity, and stability

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Carbon Energy 2021年第1期3卷 24-49页

作者： Israr Masood ul Hasan Luwei Peng Jianfeng Mao Ruiman He Yongxia Wang Jing Fu nengneng xu Jinli Qiao State Key Laboratory for Modification of Chemical Fibers and Polymer Materials College of Environmental Science and EngineeringDonghua UniversityShanghaiChina Shanghai Institute of Pollution Control and Ecological Security ShanghaiChina Institute for Superconducting and Electronic Materials Australian Institute of Innovative MaterialsUniversity of WollongongWollongongNew South WalesAustralia School of Materials Science and Engineering Tongji UniversityShanghaiChina Department of Chemical Engineering University of Louisiana at LafayetteLafayetteLouisianaUSA Institute for Materials Research and Innovation University of Louisiana at LafayetteLafayetteLouisianaUSA

Zero or negative emissions of carbon dioxide(CO2)is the need of the times,as inexorable rising and alarming levels of CO2 in the atmosphere lead to global warming and severe climate *** electrochemical CO2 reduction(eCO2R)to value‐added fuels and chemicals by using renewable electricity provides a cleaner and more sustainable route with economic benefits,in which the key is to develop clean and economical ***‐based catalyst materials possess desirable properties such as high offset potential for H2 evolution and chemical stability at the negative applied *** it is still challenging to achieve highly efficient carbon‐based catalysts,considerable efforts have been devoted to overcoming the low selectivity,activity,and ***,we summarize and discuss the recent progress in carbon‐based metal‐free catalysts including carbon nanotubes,carbon nanofibers,carbon nanoribbons,graphene,carbon nitride,and diamonds with an emphasis on their activity,product selectivity,and *** addition,the key challenges and future potential approaches for efficient eCO2R to low carbon‐based fuels are *** a good understanding of the whole history of the development of eCO2R,the CO2 reduction reactions,principles,and techniques including the role of electrolytes,electrochemical cell design and evaluation,product selectivity,and structural composition are also *** metal/metal oxides decorated with carbon‐based electrocatalysts are also *** aim to provide insights for further development of carbon‐based metal‐free electrocatalysts for CO2 reduction from the perspective of both fundamental understanding and technological applications in the future.

关键词： activity carbon‐based catalyst CO2 electrochemical reduction selectivity stability

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