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High-capacity Bi_(2)O_(3) anode for 2.4 V neutral aqueous sodium-ion battery-supercapacitor hybrid device through phase conversion mechanism

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Journal of Energy Chemistry 2022年第2期31卷 605-615页

作者： Mingze Xu Yanli Niu Xue Teng shuaiqi gong Lvlv Ji Zuofeng Chen Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China School of Materials Science and Engineering Zhejiang Sci-Tech UniversityHangzhou 310018ZhejiangChina

Aqueous battery-supercapacitor hybrid devices(BSHs)are of great importance to enrich electrochemical energy storage systems with both high energy and power ***,further improvement of BSHs in aqueous electrolytes is greatly hampered by operating voltage and capacity *** from the conventional intercalation/de-intercalation mechanism,Bi_(2)O_(3) implements charge storage by a reversible phase conversion ***,taking Bi_(2)O_(3) electrode with wide potential window(from-1.2 to 1 V *** calomel electrode)and high capacity as battery-type anode,we propose that the overall performance of aqueous BSHs can be greatly upgraded under neutral *** paring with stable layer-structuredδ-MnO_(2) cathode,a sodium-ion Bi_(2)O_(3)//MnO_(2) BSH with an ultrahigh voltage of 2.4 V in neutral sodium sulfate electrolyte is developed for the first *** hybrid device exhibits high capacity(~215 C g^(-1) at 1 mA cm^(-2)),relatively long lifespan(~77.2%capacity retention after 1500 cycles),remarkable energy density(71.7 Wh kg^(-1)@400.5 W kg^(-1))and power density(3204.3 W kg^(-1)@18.8 Wh kg^(-1)).Electrochemical measurements combining a set of spectroscopic techniques reveal the reversible phase conversion between bismuth oxide and metallic bismuth(Bi_(2)O_(3)?Bi0)through Bi^(2+) transition phase in neutral sodium sulfate solution,which can deliver multielectron transfer up to 6,leading to the high-energy *** work sheds light on the feasibility of using Bi_(2)O_(3) electrode under neutral condition to address the issue of narrow voltage and low capacity for aqueous BSHs.

关键词： Bismuth oxide Phase conversion High voltage High capacity Battery-supercapacitor hybrid devices

Upcycling PET in parallel with energy-saving H_(2)production via bifunctional nickel-cobalt nitride nanosheets

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Nano Research 2023年第4期16卷 4625-4633页

作者： Xuan Liu Zhongying Fang Dengke Xiong shuaiqi gong Yanli Niu Wei Chen Zuofeng Chen Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022China

We describe here an electro-reforming strategy to upcycle polyethylene terephthalate(PET)waste with simultaneous hydrogen production by a bifunctional nickel-cobalt nitride nanosheets *** plastics are digested in alkaline solution giving an electrochemically active monomer ethylene glycol(EG).The introduction of Co in Co-Ni3N/carbon cloth(CC)promotes the redox behavior of Ni2+/Ni3+,which is beneficial for EG oxidation at an ultra-low potential(1.15 V *** hydrogen electrode(RHE))and breaks through the limitation of high catalytic potentials of simple Ni-based electrocatalysts(1.30 V).In PET hydrolysate with Co-Ni3N/CC couples,an integrated EG oxidation-hydrogen production system achieves a current density of 50 mA·cm^(−2)at a cell voltage of 1.46 V,which is 370 mV lower than the conventional water *** in-situ Raman and Fourier transform infrared(FTIR)spectroscopies and density functional theory(DFT)calculations identify the catalytic mechanism and point to advantages of heterostructure engineering in optimizing adsorption energies and promoting catalytic activities for EG oxidation.

关键词： nickel-cobalt nitride hydrogen evolution reaction polyethylene terephthalate upcycling ethylene glycol oxidation formic acid

Paired formate and H_(2) productions via efficient bifunctional Ni-Mo nitride nanowire electrocatalysts

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Journal of Energy Chemistry 2022年第9期31卷 432-441,I0012页

作者： Xuan Liu Zhongying Fang Xue Teng Yanli Niu shuaiqi gong Wei Chen Thomas JMeyer Zuofeng Chen Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Department of Chemistry University of North Carolina at Chapel HillChapel HillNC 27599United States

Electrocatalytic water splitting provides a potentially sustainable approach for hydrogen production,but is typically restrained by kinetically slow anodic oxygen evolution reaction(OER)which is of lesser ***,free-standing,hetero-structured Ni_(3)N-Ni_(0.2)Mo_(0.8)N nanowire arrays are prepared on carbon cloth(CC)electrodes for hydrogen evolution reaction(HER)and glycerol oxidation reaction(GOR)to formate with a remarkably high Faradaic efficiency of 96%.A two-electrode electrolyzer for GOR-assisted hydrogen production operates with a current density of 10 mA cm^(-2)at an applied cell voltage of 1.40 V,220 mV lower than for alkaline water ***-situ Raman measurements identify Ni(Ⅲ)as the active form of the catalyst for GOR rather than Ni(IV)and in-situ Fourier transform infrared(FTIR)spectroscopy measurements reveal pathways for GOR to *** density functional theory(DFT)calculations,the Ni_(3)N-Ni_(0.2)Mo_(0.8)N heterostructure is beneficial for optimizing adsorption energies of reagents and intermediates and for promoting HER and GOR activities by charge redistribution across the *** same electrode also catalyzes conversion of ethylene glycol from polyethylene terephthalate(PET)plastic hydrolysate into *** combined results show that electrolytic H_(2) and formate production from alkaline glycerol and ethylene glycol solutions provide a promising strategy as a cost-effective energy supply.

关键词： Transition metal nitrides Heterostructures Hydrogen evolution reaction Glycerol and ethylene glycol oxidation Formic acid

Engineering iron-group bimetallic nanotubes as efficient bifunctional oxygen electrocatalysts for flexible Zn–air batteries

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eScience 2022年第5期2卷 546-556页

作者： Yanli Niu shuaiqi gong Xuan Liu Chen Xu Mingze Xu Shi-Gang Sun Zuofeng Chen Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai200092China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen361005China

Air cathode performance is essential for rechargeable zinc–air batteries(ZABs).In this study,we develop a self-templated synthesis technique for fabricating bimetallic alloys(FeNi_(3)),bimetallic nitrides(FeNi_(3)N)and heterostructured FeNi_(3)/FeNi_(3)N hollow *** to its structural and compositional advantages,FeNi_(3)/FeNi_(3)N exhibits remarkable bifunctional oxygen electrocatalytic performance with an extremely small potential gap of 0.68V between the oxygen evolution reaction(OER)and oxygen reduction reaction(ORR).Theoretical calculations reveal reduced Gibbs free energy for the rate-limiting O–O bond formation during OER due to the self-adaptive surface reconfiguration,which induces a synergistic effect between Fe(Ni)OOH developed in situ on the surface and the inner FeNi_(3)/FeNi_(3)*** fabricated using the FeNi_(3)/FeNi_(3)N catalyst shows high power density,small charge/discharge voltage gap and excellent cycling *** addition to its excellent battery performance,the corresponding quasi-solid-state ZAB shows robust flexibility and *** synthesis method is extended to prepare a CoFe/CoFeN oxygen electrocatalyst,demonstrating its applicability to other iron-group elements.

关键词： Bifunctional electrocatalysts Oxygen electrocatalysis Bimetallic nitrides Hollow nanotube structure Zn-air batteries

Engineering Two-Phase Bifunctional Oxygen Electrocatalysts with Tunable and Synergetic Components for Flexible Zn-Air Batteries

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Nano-Micro Letters 2021年第8期13卷 175-190页

作者： Yanli Niu Xue Teng shuaiqi gong Mingze Xu Shi-Gang Sun Zuofeng Chen Shanghai Key Laboratory of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092People’s Republic of China State Key Lab of Physical Chemistry of Solid Surface College of Chemistry and Chemical EngineeringXiamen UniversityXiamen 361005People’s Republic of China

Metal-air batteries,like Zn-air batteries(ZABs)are usually suffered from low energy conversion efficiency and poor cyclability caused by the sluggish OER and ORR at the air ***,a novel bimetallic Co/CoFe nanomaterial supported on nanoflower-like N-doped graphitic carbon(NC)was prepared through a strategy of coordination construction-cation exchange-pyrolysis and used as a highly efficient bifunctional oxygen *** characterizations and density functional theory calculations reveal the formation of Co/CoFe heterostructure and synergistic effect between metal layer and NC support,leading to improved electric conductivity,accelerated reaction kinetics,and optimized adsorption energy for intermediates of ORR and *** Co/CoFe@NC exhibits high bifunctional activities with a remarkably small potential gap of 0.70 V between the half-wave potential(E_(1/2))of ORR and the potential at 10 mA cm^(-2)(E_(j=10))of *** aqueous ZAB constructed using this air electrode exhibits a slight voltage loss of only 60 mV after 550-cycle test(360 h,15 days).A sodium polyacrylate(PANa)-based hydrogel electrolyte was synthesized with strong water-retention capability and high ionic *** quasi-solid-state ZAB by integrating the Co/CoFe@NC air electrode and PANa hydrogel electrolyte demonstrates excellent mechanical stability and cyclability under different bending states.

关键词： Bifunctional electrocatalysts Oxygen electrocatalysis Zn-air battery Co/CoFe heterointerface engineering Density functional theory calculations

碳层网络促进Sn/SnO_(2)纳米颗粒选择性CO_(2)还原

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电化学 2022年第2期28卷 113-126页

作者：滕雪牛艳丽巩帅奇刘璇陈作锋同济大学化学科学与工程学院上海200092

在各类CO_(2)还原电催化剂中,锡基材料获得了研究人员的广泛关注,但其总体催化性能仍然受催化剂电极的组成,形貌和结构的限制。在本研究中,我们利用Sn低熔点(m.p.232℃)的特性,在聚多巴胺碳化的同时实现Sn的熔化与再结晶,合成了由氮掺... 详细信息

在各类CO_(2)还原电催化剂中,锡基材料获得了研究人员的广泛关注,但其总体催化性能仍然受催化剂电极的组成,形貌和结构的限制。在本研究中,我们利用Sn低熔点(m.p.232℃)的特性,在聚多巴胺碳化的同时实现Sn的熔化与再结晶,合成了由氮掺杂碳层网络分散的异质结构Sn/SnO_(2)纳米颗粒自支撑电极(Sn/SnO_(2)@NC)。氮掺杂碳层网络有利于电子的富集,可提高催化剂电极的导电性,防止超细纳米粒子的团聚,并保护其不在电解液中溶解。在CO_(2)饱和的0.5 mol·L^(-1) NaHCO_(3)水溶液中,所制备Sn/SnO_(2)@NC电极与没有碳层网络包覆的电极相比,其CO_(2)还原催化性能得到了很大的提高。该Sn/SnO_(2)@NC电极在-0.9 V(***)的电解电压下,电流密度为17 mA·cm^(-2),甲酸盐产物的选择性为83%。通过偶联该CO_(2)还原催化电极与商品化RuO2催化剂作为水氧化阳极,可实现持续的CO_(2)/H_(2)O电解。此外,以Sn/SnO_(2)@NC为阴极,Zn箔为阳极,我们还构建了可充放电的水系Zn-CO_(2)电池。该电池的输出开路电压为1.35 V,峰值功率密度为0.9 mW·cm^(-2)。本研究为高性能CO_(2)还原催化剂的设计提供了新的思路,同时可充放电Zn-CO_(2)电池的构建为绿色能源转换和存储系统提供了新的方案。

关键词： CO_(2)电催化还原碳层网络 Sn/SnO2 甲酸 Zn-CO_(2)电池

铋基有机金属框架衍生的棒状纳米反应器用于中性水系电池型负极

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Science China Materials 2023年第1期66卷 106-117页

作者：徐铭泽巩帅奇牛艳丽张开颜刘韬陈作锋 Shanghai Key Lab of Chemical Assessment and Sustainability School of Chemical Science and EngineeringTongji UniversityShanghai 200092China

氧化铋(Bi_(2)O_(3))因其理论容量高与工作电位窗口宽而成为具有应用前景的电池型负极材料.但是,氧化铋缓慢的反应动力学与较差的循环寿命限制了其在实际器件中的应用.在本文中,我们以铋基金属有机框架(CAU-17)作为前驱体与模板,通过热... 详细信息

氧化铋(Bi_(2)O_(3))因其理论容量高与工作电位窗口宽而成为具有应用前景的电池型负极材料.但是,氧化铋缓慢的反应动力学与较差的循环寿命限制了其在实际器件中的应用.在本文中,我们以铋基金属有机框架(CAU-17)作为前驱体与模板,通过热解法结合氧化态调节制备了一种封装在棒状多孔碳纳米反应器中的Bi-Bi_(2)O_(3)纳米颗粒(Bi-Bi_(2)O_(3)@CNR).该电池型负极在硫酸钠溶液中表现出良好的导电性、快速的反应动力学、高的容量与长的循环寿命.实验结果与密度泛函理论计算表明,金属有机框架衍生的多孔碳基质与引入氧化铋晶格中的金属铋能够进一步提升氧化铋的电化学性能.基于Bi-Bi_(2)O_(3)@CNR负极和δ-MnO_(2)正极的中性水系钠离子电池电容混合器件可以同时实现高能量和高功率密度,同时具有2.4 V的超宽电位窗口.本文通过设计高稳定性和反应动力学有利的主体结构及调节活性成分的氧化态,为开发可用于中性水系电池型负极的高性能氧化铋基电极提供了新的策略.

关键词：循环寿命金属有机框架理论容量负极材料反应动力学纳米反应器硫酸钠溶液氧化铋

温度调控合成钴铁基纳米框架用于高效电催化析氧反应

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Science China Materials 2022年第2期65卷 431-441页

作者：纪律律郑慧芳韦渝洁巩帅奇王騊王晟陈作锋 School of Materials Science and Engineering Zhejiang Sci-Tech UniversityHangzhou 310018China School of Chemical Science and Engineering Tongji UniversityShanghai 200092China

过渡金属磷化物(TMPs)作为一类新型高效水分解电催化剂,近年来引起了研究人员的广泛兴趣.框架型空心纳米结构通过去除内部非功能性原子而具有独特的开放式结构,可创造更多的内部反应空间,提供丰富的活性位点和提升催化剂的原子利用率.... 详细信息

过渡金属磷化物(TMPs)作为一类新型高效水分解电催化剂,近年来引起了研究人员的广泛兴趣.框架型空心纳米结构通过去除内部非功能性原子而具有独特的开放式结构,可创造更多的内部反应空间,提供丰富的活性位点和提升催化剂的原子利用率.在本文中,我们合成了一种钴铁双金属磷化物纳米框架用于高效电催化析氧反应.该催化剂材料基于温度调控策略合成钴铁类普鲁士蓝纳米框架前驱体,随后通过磷化处理制备.实验发现,Co^(2+)和[Fe(CN)6]^(3−)共沉淀生成钴铁类普鲁士蓝前驱体的过程中,伴随反应温度从5℃升高到35℃,产物结构由实心纳米立方体转变为空心纳米框架.研究表明,纳米结构的转变与纳米立方体棱角位置的选择性外延生长相关,升高反应温度将触发前驱体分子内的电子转移并诱导结构转变.所制备的钴铁磷化物纳米框架表现出优异的电催化析氧活性,产生10 mA cm^(-2)的催化电流密度仅需276 mV的过电位,其性能优于对比样品(钴铁磷化物实心纳米立方体)和大部分近期报道的TMPs基电催化剂.本文的合成策略可拓展制备钴铁硫族化合物(如钴铁硒化物和钴铁硫化物)纳米框架,因而在能量存储与转化领域具有广泛的应用前景.

关键词：磷化处理纳米立方体开放式结构电催化剂原子利用率磷化物催化剂材料温度调控

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武德年间李世民秦王府址的变动

中国历史地理论丛 2024年第1期39卷 5-13页

作者：赵帅淇中国人民大学历史学院北京100872

武德年间李世民秦王府的方位因徐松《唐两京城坊考》的误读而模糊不清。借助吕大防《长安图》碑拓残片和《阁本太极宫图》传本等文献,可以确认武德初年至五年七月,李世民居于太极宫内西侧的承乾殿,武德五年七月之后迁至太极宫外西北方... 详细信息

武德年间李世民秦王府的方位因徐松《唐两京城坊考》的误读而模糊不清。借助吕大防《长安图》碑拓残片和《阁本太极宫图》传本等文献,可以确认武德初年至五年七月,李世民居于太极宫内西侧的承乾殿,武德五年七月之后迁至太极宫外西北方向的弘义宫。弘义宫亦为李世民发展势力、预谋政变提供了一些便利。承乾殿、弘义宫相对太子东宫都位于西方,衍生出了“西宫“”西府”等指称秦王府的概念。

关键词：秦王府承乾殿弘义宫大安宫《长安图》