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Congener-derived template to construct lithiophilic organic-inorganic layer/interphase for high volumetric capacity dendrite-free li metal batteries

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Chinese Chemical Letters 2024年第3期35卷 453-460页

作者： Kang Yang Long li yuanbin Xiao Qiaoli Zhang Chenpeng Xi Borong li Yan yu Chengkai Yang Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesCollege of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China

The development of lithium-metal batteries(LMBs)is seriously restricted by the out-of-control dendrites growth and infinite volume expansion.Herein,a pervasive organic-inorganic layer construction strategy is reported for the composite lithium metal anode with congener-derived organic-inorganic solid electrolyte interphase(SEI).In this strategy,the organic-inorganic Ag@polydopamine(Ag@PDA)layer is coated on the arbitrary substrates by a simple two-step method.The thin and stable congener-derived SEI is insitu formed with fewer inorganic components and more organic components during charging/discharging.The polydopamine with sufficient adhesion groups and lithiophilic Ag layer realize near-zero nucleation overpotential during lithium deposition.The low interface resistance and stable lithium deposition are achieved.Moreover,the practical areal and volumetric capacities of the composite anode with three-dimensional copper(3DCu)as the substrate are 10 mAh/cm^(2)and 1538 mAh/cm^3(vs.the mass of anode).The symmetrical cell shows very low polarization voltage(10 mV)and more than 2500 h cycles life at 1 mA/cm^(2)(1 mAh/cm^(2)).The liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)-based full cells show improved capacity retention(82%)after 100 cycles at 0.5 C.The modified lithiophilic anode with congener-derived interphase provides a promising strategy to realize the next-generation dendrite-free LMBs.

关键词： lithium metal anode Congener-derived lithiophilicity Volumetric capacity Organic-inorganic interphase

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Macroporous Directed and Interconnected Carbon Architectures Endow Amorphous Silicon Nanodots as Low‑Strain and Fast‑Charging Anode for lithium‑Ion Batteries

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Nano-Micro Letters 2024年第5期16卷 333-351页

作者： Zhenwei li Meisheng Han Peilun yu Junsheng lin Jie yu Guangdong Provincial Key Laboratory of Semiconductor Optoelectronic Materials and Intelligent Photonic Systems Shenzhen Engineering Lab for Supercapacitor MaterialsSchool of Material Science and EngineeringHarbin Institute of TechnologyShenzhenUniversity TownShenzhen 518055People’s Republic of China Songshan Lake Materials Laboratory Dongguan Dongguan 523808GuangdongPeople’s Republic of China Department of Mechanical and Energy Engineering Southern University of Science and TechnologyShenzhen 518055People’s Republic of China

Fabricating low-strain and fast-charging silicon-carbon composite anodes is highly desired but remains a huge challenge for lithium-ion batteries.Herein,we report a unique silicon-carbon composite fabricated by uniformly dis-persing amorphous Si nanodots(SiNDs)in carbon nanospheres(SiNDs/C)that are welded on the wall of the macroporous carbon framework(MPCF)by vertical graphene(VG),labeled as MPCF@VG@SiNDs/C.The high dispersity and amor-phous features of ultrasmall SiNDs(~0.7 nm),the flexible and directed electron/li+transport channels of VG,and the MPCF impart the MPCF@VG@SiNDs/C more lithium storage sites,rapid li+transport path,and unique low-strain property during li+storage.Consequently,the MPCF@VG@SiNDs/C exhibits high cycle stability(1301.4 mAh g^(-1) at 1 A g^(-1) after 1000 cycles without apparent decay)and high rate capacity(910.3 mAh g^(-1),20 A g^(-1))in half cells based on industrial electrode standards.The assembled pouch full cell delivers a high energy density(1694.0 Wh L^(-1);602.8 Wh kg^(-1))and an excellent fast-charging capability(498.5 Wh kg^(-1),charging for 16.8 min at 3 C).This study opens new possibilities for preparing advanced silicon-carbon com-posite anodes for practical applications.

关键词： Amorphous Si nanodots Low-strain Fast-charging lithium-ion batteries

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Optimal geometrical configuration and oxidation state of cobalt cations in spinel oxides to promote the performance of li-O_(2) battery

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Nano Research 2024年第1期17卷 221-227页

作者： yu Zhang Shuting Zhang Mengwei yuan yufeng li Rong liu Caiyun Nan Chen Chen Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084China Beijing Key Laboratory of Energy Conversion and Storage Materials Institution College of ChemistryBeijing Normal UniversityBeijing 100875China X-ray diffraction Lab Analytical and Testing CenterBeijing Normal UniversityBeijing 100875China

Co_(3)O_(4) is considered as one of promising cathode catalysts for lithium oxygen(li-O_(2))batteries,which contains both tetrahedral Co^(2+)sites(Co^(2+)Td)and octahedral Co^(3+)sites(Co^(3+)Oh).It is important to reveal the effect of optimal geometric configuration and oxidation state of cobalt ion in Co_(3)O_(4) to improve the performance of li-O_(2) batteries.Herein,through regulating the synthesis process,Co^(2+)and Co^(3+)sites in Co_(3)O_(4) were replaced with Zn and Al atoms to form materials with a unique Co site.The li-O_(2) batteries based on ZnCo_(2)O_(4) showed longer cycle life than that of CoAl_(2)O_(4),suggesting that in Co_(3)O_(4),the Co^(3+)Oh site is a relatively better geometric configuration than Co^(2+)Td site for li-O_(2) batteries.Theoretical calculations revealed that Co^(3+)Oh sites provide higher catalysis activity,regulating the adsorption energy of the intermediate liO_(2) and accelerating the kinetics of the reaction in batteries,which further leads to the change of the morphology of the discharge product and ultimately improves the electrochemical performance of the batteries.

关键词： lithium oxygen(li-O_(2))batteries geometrical configuration oxidation state lithium peroxide

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Exploring changes of precipitation extremes under climate change through global variable-resolution modeling

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Science Bulletin 2024年第2期69卷 237-247页

作者： Wei Sun Jian li Rucong yu Nina li Yi Zhang State Key Laboratory of Severe Weather Chinese Academy of Meteorological SciencesBeijing 100081China Institute of Tibetan Plateau Meteorology China Meteorological AdministrationChengdu 610072China Department of Atmospheric Science Yunnan UniversityKunming 650091China National Meteorological Center China Meteorological AdministrationBeijing 100081China 2035 Future Laboratory PIESAT Information Technology Co.Ltd.Beijing 100105China

Understanding the responses of precipitation extremes to global climate change remains limited owing to their poor representations in models and complicated interactions with multi-scale systems.Here we take the record-breaking precipitation over China in 2021 as an example,and study its changes under three different climate scenarios through a developed pseudo-global-warming(PGW)experimental framework with 60-3 km variable-resolution global ensemble modeling.Compared to the present climate,the precipitation extreme under a warmer(cooler)climate increased(decreased)in intensity,coverage,and total amount at a range of 24.3%-37.8%(18.7%-56.1%).With the help of the proposed PGW experimental framework,we further reveal the impacts of the multi-scale system interactions in climate change on the precipitation extreme.Under the warmer climate,large-scale water vapor transport converged from double typhoons and the subtropical high marched into central China,enhancing the convective energy and instability on the leading edge of the transport belt.As a result,the mesoscale convective system(Mcs)that directly contributed to the precipitation extreme became stronger than that in the present climate.On the contrary,the cooler climate displayed opposite changing characteristics relative to the warmer climate,ranging from the large-scale systems to local environments and to the Mcs.In summary,our study provides a promising approach to scientifically assess the response of precipitation extremes to climate change,making it feasible to perform ensemble simulations while investigating the multi-scale system interactions over the globe.

关键词： Precipitation extreme Climate change Pseudo-global-warming experiment Variable-resolution modeling Multi-scale system interaction

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Integration of urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays within porous copper current collector for superior performance li-ion battery anodes

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Rare Metals 2024年第2期43卷 599-611页

作者： Xue-Ru Zhang Qiong Wu Yong Zhang Xi-Fei li Ting Xie yu-Cheng Wu Instrumental Analysis Center Hefei University of TechnologyHefei230009China Key Laboratory of Advanced Functional Materials and Devices of Anhui Province Hefei230009China School of Materials Science and Engineering Hefei University of TechnologyHefei230009China Institute of Advanced Electrochemical Energy Xi’an University of TechnologyXi’an710048China

Spinel MnCo_(2)O_(4) is a promising energy storage candidate as anode materials in lithium-ion batteries owing to synergistic effects of two intrinsic solid-state redox couples.However,low conductivity,poor rate capacity and rapid capacity fading have seriously impaired its practical applications.To overcome the inferiorities,urchin-like MnCo_(2)O_(4)@C core–shell nanowire arrays have been fabricated directly within a porous copper current collector via a facile hydrothermal method followed by a chemical vapor deposition carbonization process.In a typical nanowire,the core is composed of interconnected MnCo_(2)O_(4)nanoparticles and the shell shows as a thin amorphous carbon layer.The integrated MnCo_(2)O_(4)@C/Cu structure could act as working anodes without using additives or polymer binders.While MnCo_(2)O_(4)@C/Cu possesses slightly longer li-ion insertion/desertion pathway than that of MnCo_(2)O_(4)/Cu,the carbon shell could effectively prevent the pulverization of MnCo_(2)O_(4) and lower down charge transfer resistance and actively participate in li-ion cycles.The rearrangement of carbon atoms during lithiation/delithiation cycling could inhibit the formation of passive solid electrolyte interphase films.As a result,the MnCo_(2)O_(4)@C/Cu electrode presents superior rate capacity(600 mAh·g^(−1) at 1 A·g^(−1)) and better stability(797 mAh·g^(−1) after 200 cycles at 100 mA·g^(−1)).The excellent reversible li ion storage capacity,cycling stability and rate capacity endow MnCo_(2)O_(4)@C/Cu great potential as stable and high output integrated anode materials in li-ion batteries.

关键词： MnCo_(2)O_(4)@C Urchin-like nanowire arrays Core-shell Integrated anode materials lithium-ion batteries

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Highly-chlorinated inert and robust interphase without mineralization of oxide enhancing high-rate li metal batteries

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Chinese Chemical Letters 2024年第6期35卷 239-243页

作者： Long li Kang Yang Chenpeng Xi Mengchao li Borong li Gui Xu yuanbin Xiao Xiancai Cui Zhiliang liu lingyun li Yan yu Chengkai Yang Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesSchool of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China College of Material Sciences and Chemical Engineering Harbin Engineering UniversityHarbin 150001China

Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries.In this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient li metal anode.The polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional theory.The organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as li_(2)O and li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and liFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.

关键词： Highly-chlorinated Water/oxygen resistance Stable interphase Dendrite-free lithium metal batteries High-rate

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NbN quantum dots anchored hollow carbon nanorods as efficient polysulfide immobilizer and lithium stabilizer for li-S full batteries

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Journal of Energy Chemistry 2024年第1期88卷 260-271,I0007页

作者： Fei Ma Zhuo Chen Katam Srinivas Ziheng Zhang yu Wu Dawei liu Hesheng yu yue Wang Xinsheng li Ming-qiang Zhu Qi Wu yuanfu Chen School of Integrated Circuit Science and Engineering and State Key Laboratory of Electronic Thin Films and Integrated DevicesUniversity of Electronic Science and TechnologyChengdu 610054SichuanChina College of Science and Institute of Oxygen Supply Center of Tibetan Studies(Everest Research Institute)Tibet UniversityLhasa 850000TibetChina College of Mechanical and Electronic Engineering Northwest A&F UniversityXianyang 712100ShaanxiChina

The shuttle effect of lithium polysulfides(liPSs)and uncontrollable lithium dendrite growth seriously hinder the practical application of lithium-sulfur(li-S)batteries.To simultaneously address such issues,monodispersed Nb N quantum dots anchored on nitrogen-doped hollow carbon nanorods(NbN@NHCR)are elaborately developed as efficient li PSs immobilizer and li stabilizer for high-performance li-S full batteries.Density functional theory(DFT)calculations and experimental characterizations demonstrate that the sulfiphilic and lithiophilic NbN@NHCR hybrid can not only efficiently immobilize the soluble li PSs and facilitate diffusion-conversion kinetics for alleviating the shuttling effect,but also homogenize the distribution of li+ions and regulate uniform li deposition for suppressing li-dendrite growth.As a result,the assembled li-S full batteries(NbN@NHCR-S||Nb N@NHCR-li)deliver excellent long-term cycling stability with a low decay rate of 0.031%per cycle over 1000 cycles at high rate of 2 C.Even at a high S loading of 5.8 mg cm^(-2)and a low electrolyte/sulfur ratio of 5.2μL mg^(-1),a large areal capacity of 6.2 mA h cm^(-2)can be achieved in li-S pouch cell at 0.1 C.This study provides a new perspective via designing a dual-functional sulfiphilic and lithiophilic hybrid to address serious issues of the shuttle effect of S cathode and dendrite growth of li anode.

关键词： Dual-functional host NbN quantum dots Shuttle effect Dendrite-free li anode li-S full batteries

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Pd cluster decorated free standing flexible cathode for high performance li-oxygen batteries

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Nano Research 2024年第4期17卷 2678-2686页

作者： liang Guo Guoliang Zhang Ruonan Yang Dongmei Zhang Xiuqi Zhang Han yu Xia li Feng Dang Key Laboratory for liquid-Solid Structure Evolution and Processing of Materials Ministry of EducationShandong UniversityJinan 250061China

As a promising candidate for the next generation energy storage system,rechargeable lithium-oxygen batteries(LOBs)still face substantial challenges caused by insulating discharge products that preclude their practical application.Exploring highly efficient cathode catalysts capable of facilitating formation/decomposition of discharge products is considered as an essential approach towards high performance LOBs.Herein,Pd decorated Te nanowires(Pd@Te NWs)were synthesized as advanced catalyst in LOBs to maximize Pd utilization and achieve synergistic effect,in which Pd clusters were uniformly grown on Te substrate though regulating the Pd:Te ratio.Meanwhile,Pd@Te nanowires assembled into an interpenetrating network-like structure by vacuum filtration and employed as flexible cathode,enabling LOBs achieved an ultralong 190 cycles stability and a superior specific capacity of 3.35 mAh·cm^(-2).Experimental studies and density functional theory(DFT)calculations reveal the excellent catalytic ability of Pd@Te and synergistic catalytic mechanism of Pd and Te,in which uniform electron distribution,extensive electron exchange,and large adsorption distance between Pd cluster and discharge products promote homogeneous adsorption/desorption of discharge products,while the high adsorption energy of Te substrate for li species reduces the initial dynamical energy barrier during discharging process.The current work provides viable strategy to design composite catalysts for flexible cathode of LOBs with synergistic catalytic effects.

关键词： flexible lithium-oxygen batteries Pd@Te synergistic catalysis cathode catalysts density functional theory(DFT)calculation

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Three-stage niobium mineralization at Bayan Obo, China

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National Science Review 2024年第4期11卷 102-110页

作者： Yan yu Yang li yu liu Xiao-Xiao ling li-Guang Wu li Yang Lan Yang Bo Yang Yong-Gang Zhao Xian-Hua li State Key Laboratory of lithospheric Evolution Institute of Geology and Geophysics Chinese Academy of Sciences College of Earth and Planetary Science University of Chinese Academy of Sciences Ministry of Education Key Laboratory of Orogenic Belts and Crustal Evolution School of Earth and Space SciencesPeking University Mining Research Institute Baotou Iron and Steel(Group) Co.LTD State Key Laboratory of Baiyunobo Rare Earth Resource Research and Comprehensive Utilization

The Chinese Bayan Obo deposit is a world-class rare earth element(REE) deposit with considerable niobium(Nb) and iron(Fe) resources. A complete genetic understanding on all metals is fundamental for establishing genetic models at Bayan Obo. With extensive research being focused on REE enrichment, the timing and controls of Nb enrichment remain unresolved at Bayan Obo, which is mainly due to the challenges in dating, i.e. multistage thermal events, fine-grained minerals with complex textures and the rare occurrence of uranium-enriched minerals with mature dating methods. Based on robust geological and petrographic frameworks, here we conducted ion probe uranium-lead(U-Pb) dating of ferrocolumbite to unravel the timing, hence the genesis of Nb mineralization. Three types of hydrothermal ferrocolumbites—key Nb-bearing minerals—are identified based on their textures and mineral assemblages. They yield U-Pb ages of 1312 ± 47 Ma(n = 99), 438 ± 7 Ma(n = 93), and 268 ± 5 Ma(n = 19), respectively. In line with deposit geology, we tentatively link the first, second and third stage Nb mineralization to Mesoproterozoic carbonatite magmatism, ubiquitous early Paleozoic hydrothermal activity, and Permian granitic magmatism, respectively. While quantifying the contribution of metal endowment from each stage requires further investigation, our new dates highlight that multi-stage mineralization is critical for Nb enrichment at Bayan Obo, which may also have implications for the enrichment mechanism of Nb in REE deposits in general.

关键词： niobium mineralization U-Pb dating ferrocolumbite Bayan Obo

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Quantum Spin Exchange Interactions to Accelerate the Redox Kinetics in li–S Batteries

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Nano-Micro Letters 2024年第5期16卷 370-383页

作者： yu Du Weijie Chen yu Wang yue yu Kai Guo Gan Qu Jianan Zhang Key Laboratory of Advanced Energy Catalytic and Functional Materials Preparation of Zhengzhou City College of Materials Science and EngineeringZhengzhou UniversityZhengzhou 450001People’s Republic of China

Spin-engineering with electrocatalysts have been exploited to suppress the“shuttle effect”in li–S batteries.Spin selec-tion,spin-dependent electron mobility and spin potentials in activation barriers can be optimized as quantum spin exchange interactions lead-ing to a significant reduction of the electronic repulsions in the orbitals of catalysts.Herein,we anchor the MgPc molecules on fluorinated carbon nanotubes(MgPc@FCNT),which exhibits the single active Mg sites with axial displacement.According to the density functional theory calculations,the electronic spin polarization in MgPc@FCNT not only increases the adsorption energy toward liPSs intermediates but also facilitates the tunneling process of electron in li–S batter-ies.As a result,the MgPc@FCNT provides an initial capacity of 6.1 mAh cm^(-2) even when the high sulfur loading is 4.5 mg cm^(-2),and still maintains 5.1 mAh cm^(-2) after 100 cycles.This work provides a new perspective to extend the main group single-atom catalysts enabling high-performance li–S batteries.

关键词： Metal phthalocyanines Spin polarization Electrocatalysis li–S batteries

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