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Nano Research 2024年第6期17卷 5179-5187页

作者： Jinlei Qin Rui Wang Zilong Yuan Pei Xiao Deli Wang key laboratory of Material Chemistry for energy Conversion and Storage Ministry of EducationHubei Key Laboratory of Material Chemistry and Service FailureSchool of Chemistry and Chemical EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Lithium-sulfur(Li-S)batteries have been considered as promising energy storage systems due to the merits of high energy density and low cost.However,the lithium polysulfides(LiPSs)diffusion and sluggish redox kinetics hamper the battery performance.In this work,low-bandgap indium oxide(In_(2)O_(3))with dense oxygen vacancies(In_(2)O_(3−x),0

关键词： Li-S batteries nitrogen-doped carbon confinement oxygen vacancies bidirectional Li_(2)S redox

A case study of comparing two dimerized acceptor molecules built by different branch-connected and terminal-connected approaches

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Science China Chemistry 2024年第5期67卷 1687-1696页

作者： Kangqiao Ma Huazhe Liang Yuxin Wang Tengfei He Tainan Duan Xiaodong Si Wendi Shi Guankui Long Xiangjian Cao Zhaoyang Yao Xiangjian Wan Chenxi Li Bin Kan Yongsheng Chen State key laboratory and Institute of Elemento-Organic Chemistry Frontiers Science Center for New Organic MatterThe Centre of Nanoscale Science and Technology and Key Laboratory of Functional Polymer MaterialsInstitute of Polymer ChemistryRenewable Energy Conversion and Storage Center(RECAST)College of ChemistryNankai UniversityTianjin 300071China School of Materials Science and Engineering National Institute for Advanced MaterialsRenewable Energy Conversion and Storage Center(RECAST)Nankai UniversityTianjin 300350China Chongqing Institute of Green and Intelligent Technology Chongqing SchoolUniversity of Chinese Academy of Sciences(UCAS Chongqing)Chinese Academy of SciencesChongqing 400015China

Dimerized small-molecule acceptors(SMAs) built by the conventional connection of terminal groups of monomers have contributed to exciting long-term stabilities of organic solar cells(OSCs). However, device efficiencies, especially fill factors(FFs), still need to be improved. This probably originates from unsymmetrical molecular structure/conformation-determined less compact/ordered molecular stackings, such as ineffective stackings of constraint terminals. Herein, an exotic dimerized SMA of BC-Th is established by bridging the branched groups(BC-type, branch coupling) of two monomers rather than conventional terminal units(TC-type, terminal coupling). Benefiting from the three-dimensional conformation and more uncurbed terminals,BC-Th exhibits multiple molecular orientations along with a larger dielectric constant and electron mobility compared with TCTh. Finally, an efficiency of 17.43% is achieved by BC-Th-based OSCs, along with the highest FF of 79.13% among all dimerized SMAs-based OSCs to date. When introducing L8-BO as the third component, overall enhanced efficiency of 18.05%and FF of 80.11% are further afforded. Contrarily, TC-Th-based OSCs exhibit much inferior PCE of 16.29% and FF of 74.81%,demonstrating the great advantages of “branch coupling” over “terminal coupling” when building dimerized SMAs.

关键词： organic solar cells dimerized acceptor molecules branch coupling morphology control stability

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng key laboratory of Automobile Materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

Atomization characteristics of pyrolysis oil derived from waste tires

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Waste Disposal and Sustainable energy 2024年第1期6卷 39-52页

作者： Hong Feng Zhitong Yin Qin Hong Yiming Hu Lintao Liu Jun Wang Qunxing Huang Yonggang Zhou ZJMI Environmental energy Co. LtdHangzhou310003China Tongxiang Taiaisi Environmental Protection energy Co. Ltd.Jiaxing314500China State key laboratory of Clean energy Utilization Zhejiang UniversityHangzhou310027China key laboratory of Clean energy and Carbon Neutrality of Zhejiang Province Jiaxing Research InstituteZhejiang UniversityJiaxing314031China

The atomization characteristics play a key role in the highly efficient combustion of pyrolysis oil derived from waste tires.In this study,the fuel properties of tire pyrolysis oil(TPO)were initially studied,and then a high-speed camera and a phase Doppler particle analyzer were employed to characterize the atomization feature of TPO.The influence of pressure and nozzle orifice diameter on atomization characteristics such as spray angle,droplet velocity,and droplet size distribution was investigated.The results showed that TPO had a high calorific value of about 43.6 MJ/kg and a low viscosity of 3.84×10^(–6)m^(2)/s at 40℃,which made it have the potential to be used as an alternative fuel.Higher pressure expanded the spray angle and extended the spray in both the axial and radial directions.With increasing pressure,spray angle and droplet velocity raised,and the increase in crushing effect of air reduced the Sauter mean diameter(SMD)of the droplets.To obtain proper atomization quality for combustion,the pressure is expected to be higher than 1.25 MPa.With increasing nozzle orifice diameter,droplet velocity increased,and the SMD of the droplets increased as well due to weakened crushing effect of the orifice.Therefore,the pressure must be increased to maintain the atomization quality when using a nozzle with a larger orifice.Due to the lower viscosity,the velocity and particle size distribution of TPO droplets after atomization were smaller than those of diesel droplets.The extremely small carbon black contained in TPO also contributed to the breaking of droplets and played a certain role in the size reduction of the oil droplets,but it may cause the risk of nozzle blockage.In summary,TPO showed great atomization characteristics for alternative fuel applications.

关键词： Pyrolysis oil Atomization characteristics Spray angle Droplet velocity Droplet size distribution

Regulating electrochemical performances of lithium battery by external physical field

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Rare Metals 2024年第6期43卷 2391-2417页

作者： Shi-Kang Wang Shuai Wu Yi-Cheng Song Hassanien Gomaa Cui-Hua An Qi-Bo Deng Ning Hu School of Mechanical Engineering School of Materials Science and EngineeringHebei University of Technology Shanghai key laboratory of Mechanics in energy Engineering Department of Chemistry Faculty of ScienceAl-Azhar University Tianjin key laboratory of Power Transmission and Safety Technology for New energy Vehicles State key laboratory of Reliability and Intelligence Electrical Equipment Key Laboratory of Advanced Intelligent Protective Equipment TechnologyMinistry of EducationHebei University of Technology

Lithium batteries have always played a key role in the field of new energy sources.However,non-controllable lithium dendrites and volume dilatation of metallic lithium in batteries with lithium metal as anodes have limited their development.Recently,a large number of studies have shown that the electrochemical performances of lithium batteries can be enhanced through the regulation of external physical fields.Especially,it significantly hinders the growth of lithium dendrites and promoting the reaction kinetics.This review summarizes recent innovations in the investigation of various physical fields of lithium batteries.The application of magnetic field in the synthesis of lithium battery electrode materials is introduced.The influence factors and regulation mechanism of various physical fields on the electrochemical performance of lithium batteries are reviewed emphatically.In addition,the current research status and existing challenges,along with future directions for the evolution of lithium batteries,are minutely discussed and prospected.New strategies for the further evolution of lithium batteries have also been provided.

关键词： Lithium battery External field assist Reaction kinetics Lithium dendrite

Highly sensitive fluorescent sensing and photocatalytic degradation performance of two-dimensional Tb-organic network

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Journal of Rare Earths 2024年第2期42卷 303-313,I0003页

作者： Ting Gao Zhihu Ma Yixia Ren Zhixiang Wang Meili Zhang Xiaoli Chen Jijiang Wang laboratory of New energy and New Function Materials Shaanxi Key Laboratory of Chemical Reaction EngineeringCollege of Chemistry and Chemical EngineeringYan'an UniversityYan'an716000China

A novel tetra-nuclear Tb-organic network,named as [Tb_(4)(2-pyia)_(6)(HAc)_(0.5)(2,2'-bipy)(H_(2)O)_(4.5)]·2,2'-bipy·H_(2)O(1),was synthesized hydrothermally based on 5-(pyridin-2-ylmethoxy) isophthalic acid(H_(2)pyia) and 2,2'-bipyridine(2,2'-bipy) ligands,and characterized by single crystal X-ray diffraction,thermogravimetric(TG) analyses,powder X-ray diffraction(PXRD) and infrared(IR) technology.1 possesses a two-dimensional network based on the tetra-nuclear inorganic building units,and the π-πstacking interactions between the pyia^(2-) ligands and the guest 2,2'-bipy molecules play an important role in the forming of 3D supramolecular structure.1 exhibits excellent fluorescent sensing performance for Fe^(3+)(1.26×10^(-8) mol/L),Cr_(2)O_(7)^(2-)(8.1×10^(-7) mol/L),2,4,6-trinitrophenol(TNP)(2.71×10^(-8) mol/L)and tetracycline(TCT)(2.76×10^(-7) mol/L) in aqueous solution with lower detection concentrations.The sensing mechanisms of 1 were investigated by density functional theory(DFT) calculations,ultraviolet-visible(UV-Vis) diffuse reflectance spectroscopy,PXRD and fluorescent lifetime analyses.The activated product of 1 was prepared by heating at 255℃ under constant pressure and used to photo-catalytically degrade TCT.Both 1 and the activated one have good photocatalytic degradation performance for TCT with degradation rates of 84.29% and 96.07%,respectively.The photocatalytic mechanisms were discovered by UV-Vis diffuse reflectance spectroscopy and radical trap experiments.The Tb-organic framework might be an excellent multifunctional fluorescent sensor and a good photocatalytic agent for TCT degradation in the future.

关键词： Tb-organic network Fluorescent sensing Photocatalytic degradation Rare earths

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A small organic molecule strategy for remedying oxygen vacancies by bismuth defects in BiOBr nanosheet with excellent photocatalytic CO_(2)reduction

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Nano Research 2024年第1期17卷 297-306页

作者： Jing Xie Zhenjiang Lu Yue Feng Jianguo Huang Jindou Hu Aize Hao Yali Cao State key laboratory of Chemistry and Utilization of Carbon Based energy Resources College of ChemistryXinjiang UniversityUrumqi 830046China

Defect modulation currently plays a decisive role in addressing the poor photoabsorption,sluggish electron hole separation,and high CO_(2)activation barrier in photocatalytic CO_(2)reduction.However,hunting for a straightforward strategy to balance the concentration of oxygen vacancy and metal cation defect in one photocatalyst is still a great challenge.Herein,a bismuth vacancies BiOBr nanosheets(BiOBr-1)on the exposed[001]facets were constructed via an acetic acid molecule modification strategy,which can repair oxygen defect by bismuth vacancy in low-temperature solid-state chemical method.Benefiting from the formed bismuth defects that can not only broaden light absorption and elevate charge separation efficiency,but also enhance adsorption and activation of CO_(2)molecules,the evolution rates of photocatalytic CO_(2)conversion into CO(71.23μmol·g^(-1)·h^(-1))and CH4(8.90μmol·g^(-1)·h^(-1))attained by BiOBr-1 are superior 7.1 and 11 times to that of plate-like BiOBr.The photocatalytic mechanisms including adsorption concentration and activation process of CO_(2)are further revealed by the in situ diffuse reflectance infrared flourier transform spectra(DRIFTS).This finding of the existence of distinct defects in ultrathin nanosheets undoubtedly leads to new possibilities for photocatalyst design using two-dimensional materials with high solar-driven photocatalytic activity.

关键词： solid-state synthesis BiOBr metal vacancies photocatalysis carbon dioxide reduction

Cobalt-doped TiO_(2)@C hierarchical nanocomposites derived from Ti_(3)C_(2) MXene as cathodes for hybrid magnesium-lithium batteries

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Nano Research 2024年第1期17卷 253-261页

作者： Xiaohui Li Yakun Tang Lang Liu Yue Zhang Yang Gao Mao Qian Wenjie Ma State key laboratory of Chemistry and Utilization of Carbon Based energy Resources College of ChemistryXinjiang UniversityUrumqi 830017China

TiO_(2)has been explored in hybrid magnesium-lithium batteries(HMLBs)due to the advantages of low self-discharge and small volume expansion during ion insertion.However,how to improve the inherently low ionic and electrical conductivity of TiO_(2)is the problem that needs to be solved.In this work,a smart strategy is adopted to prepare cobalt-doped TiO_(2)@C(Co^(4+)-TiO_(2)@C)hierarchical nanocomposite derived from Co(II)(OH)n@Ti3C2.Compared with TiO_(2)@C(without cobalt doping),Co^(4+)-TiO_(2)@C shows the highest specific capacity(154.7 mAh·g^(-1)at 0.1 A·g^(-1)after 200 cycles)and extraordinary rate performance in HMLBs.The excellent electrochemical performance of Co4+-TiO_(2)@C is ascribed to the synergistic effect of the hierarchical structure and cobalt-doping.Both experimental results and density functional theory(DFT)calculation reveal that the cobalt-doping has effectively improved the electronic conductivity and reduced the Li+migration barrier.This work provides a new insight to design TiO_(2)-based cathode materials with high-performance in HMLBs.

关键词： Ti_(3)C_(2)MXene TiO_(2) hybrid magnesium-lithium batteries hierarchical structure cobalt-doping

Solvation Engineering via Fluorosurfactant Additive Toward Boosted Lithium-Ion Thermoelectrochemical Cells

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Nano-Micro Letters 2024年第4期16卷 253-268页

作者： Yinghong Xu Zhiwei Li Langyuan Wu Hui Dou Xiaogang Zhang Jiangsu key laboratory of Electrochemical energy Storage Technologies College of Material Science and TechnologyNanjing University of Aeronautics and AstronauticsNanjing 211106People’s Republic of China

Lithium-ion thermoelectrochemical cell(LTEC), featuring simultaneous energy conversion and storage, has emerged as promising candidate for low-grade heat harvesting. However, relatively poor thermosensitivity and heat-to-current behavior limit the application of LTECs using LiPF_6 electrolyte. Introducing additives into bulk electrolyte is a reasonable strategy to solve such problem by modifying the solvation structure of electrolyte ions. In this work, we develop a dual-salt electrolyte with fluorosurfactant(FS) additive to achieve high thermopower and durability of LTECs during the conversion of low-grade heat into electricity. The addition of FS induces a unique Li~+ solvation with the aggregated double anions through a crowded electrolyte environment,resulting in an enhanced mobility kinetics of Li~+ as well as boosted thermoelectrochemical performances. By coupling optimized electrolyte with graphite electrode, a high thermopower of 13.8 mV K^(-1) and a normalized output power density of 3.99 mW m^(–2) K^(–2) as well as an outstanding output energy density of 607.96 J m^(-2) can be obtained.These results demonstrate that the optimization of electrolyte by regulating solvation structure will inject new vitality into the construction of thermoelectrochemical devices with attractive properties.

关键词： Solvation engineering Fluorosurfactant Ionic thermoelectric Lithium-ion thermoelectrochemical cell Low-grade heat

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Introducing sulfur to nickel-iron selenide for high-efficiency alkaline seawater electrolysis

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Science China Chemistry 2024年第8期67卷 2747-2754页

作者： Xuanwa Chen Yanhui Yu Xingqi Han Huan Wang Yingjie Hua Daoxiong Wu Peilin Deng Juanxiu Xiao Xinlong Tian Jing Li School of Marine Science and Engineering Hainan Provincial Key Lab of Fine Chemistry School of Chemistry and Chemical EngineeringHainan University key laboratory of Advanced energy Materials Chemistry (Ministry of Education) College of Chemistry Nankai University key laboratory of Electrochemical energy Storage and energy Conversion of Hainan Province School of Chemistry and Chemical Engineering Hainan Normal University

Seawater electrolysis is an effective way to obtain hydrogen（H2） in a sustainable manner. However, the lack of electrocatalysts with high activity, stability, and selectivity for oxygen evolution reaction（OER） severely hinders the development of seawater electrolysis technology. Herein, sulfur-doped nickel-iron selenide nanosheets（S-NiFeSe2） were prepared by an ion-exchange strategy and served as highly active OER electrocatalyst for alkaline seawater electrolysis. The overpotential is 367 m V, and it can run stably for over 50 h at 100 m A cm-2. Excitingly, the S-NiFeSe2||Pt/C pair exhibits cell voltage of 1.54 V at 10 m A cm-2under alkaline seawater conditions, which can run smoothly for 100 h without decay, and the efficiency of electricity-tohydrogen（ETH） energy conversion reaches more than 80%. Such electrode, with abundant accessible reactive sites and good corrosion resistance, is a good candidate for seawater electrolysis. Moreover, density functional theory calculations reveal that the surface sulfur atoms can activate the adjacent Ni sites and decrease the free energy changes of the associated intermediates at the adjacent Ni sites for OER, and the step of*OH →*O is the potential rate-limiting step. In this work, the true reactive site in nickel-iron selenides is the Ni sites, but not the Fe sites as commonly believed.

关键词： alkaline seawater electrolysis electrocatalysts nickel-iron selenide oxygen evolution reaction S-doping