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Efficient anion immobilization enabled by structurally controllable halloysite for dendrite-free sodium metal anode

中国科学:化学英文版 2023年第9期66卷 2600-2611页

作者： Caihong Yang Yicheng Hua Ying Zhang Jie Wang Huanwen Wang Liangjie Fu Aidong Tang Huaming Yang Engineering Research Center of Nano-Geomaterials of Ministry of Education China University of GeosciencesWuhan 430074China Laboratory of Advanced Mineral Materials China University of GeosciencesWuhan 430074China Faculty of Materials Science and Chemistry China University of GeosciencesWuhan 430074China College of Chemistry and Chemical Engineering Central South UniversityChangsha 410083China Hunan Key Laboratory of Mineral Materials and Application School of Minerals Processing and BioengineeringCentral South UniversityChangsha 410083China

Sodium metal has shown great potential as an inexpensive anode for rechargeable batteries. However, the growth of sodium dendrites continues to hinder the commercialization of Na metal batteries. Herein, an effective strategy using anion-anchoring halloysite nanotube(HNT) coating was proven to prevent the diffusion of anions and trigger uniform Na deposition. Through theoretical calculation, a model of active site of fixed anions exposed from HNTs after acid activation was established for the first time, revealing that Si–Al sites are effective active site of acid-activated HNTs. Furthermore, HNTs with strong and effective adsorption capacity for anions were obtained by controlling the structure of HNTs to regulate the exposure of Si–Al sites. The strong interaction between sites of acid-activated HNTs and the SO_(3)CF_(3)^(-) anion effectively promotes the dissociation of sodium salts, the release of Na^(+) and subsequent migration. As a result, HNTs acid activation for 4 h shows a steady sodium deposition process and displays high Coulombic efficiency in half cell, long cycle life in symmetric cell and full cell. This work provides a basic theoretical basis for the design of nanoclay with abundant and effective active site to fix anions for dendritic free metal batteries.

关键词： halloysite anion immobilization ion transport sodium dendrites sodium metal batteries

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Revealing alkali metal ions transport mechanism in the atomic channels of Au@a-MnO_(2)

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Journal of Energy Chemistry 2023年第7期82卷 350-358,I0008页

作者： Jingzhao Chen Yong Su Hongjun Ye Yushu Tang Jitong Yan Zhiying Gao Dingding Zhu Jingming Yao Xuedong Zhang Tingting Yang Baiyu Guo Hui Li Qiushi Dai Yali Liang Jun Ma Bo Wang Haiming Sun Qiunan Liu Jing Wang Congcong Du Liqiang Zhang Yongfu Tang Jianyu Huang Clean Nano Energy Center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066004HebeiChina School of Materials Science and Engineering Xiangtan UniversityXiangtan 411105HunanChina Hebei Key Laboratory of Applied Chemistry College of Environmental and Chemical EngineeringYanshan UniversityQinhuangdao 066004HebeiChina

Understanding alkali metal ions’(e.g.,Li^(+)/Na^(+)/K^(+))transport mechanism is challenging but critical to improving the performance of alkali metal batteries.Herein using a-MnO_(2)nanowires as cathodes,the transport kinetics of Li^(+)/Na^(+)/K^(+)in the 2×2 channels of a-MnO_(2)with a growth direction of[001]is revealed.We show that ion radius plays a decisive role in determining the ion transport and electrochemistry.Regardless of the ion radii,Li^(+)/Na^(+)/K^(+)can all go through the 2×2 channels of a-MnO_(2),generating large stress and causing channel merging or opening.However,smaller ions such as Li^(+)and Na^(+)cannot only transport along the[001]direction but also migrate along thedirection to the nanowire surface;for large ion such as K^(+),diffusion along thedirection is prohibited.The different ion transport behavior has grand consequences in the electrochemistry of metal oxygen batteries(MOBs).For Li-O_(2)battery,Li^(+)transports uniformly to the nanowire surface,forming a uniform layer of oxide;Na^(+)also transports to the nanowire surface but may be clogged locally due to its larger radius,therefore sporadic pearl-like oxides form on the nanowire surface;K^(+)cannot transport to the nanowire surface due to its large radius,instead,it breaks the nanowire locally,causing local deposition of potassium oxides.The study provides atomic scale understanding of the alkali metal ion transport mechanism which may be harnessed to improve the performance of MOBs.

关键词： ion transport In-situ TEM STEM Metal oxygen batteries Metal ion batteries

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The Transference Number

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Energy & Environmental Materials 2022年第2期5卷 366-369页

作者： Kevin W.Gao Chao Fang David M.Halat Aashutosh Mistry John Newman Nitash P.Balsara Materials Sciences Division Lawrence Berkeley National LaboratoryBerkeleyCA 94720USA Department of Chemical and Biomolecular Engineering University of CaliforniaBerkeleyCA 94720USA Joint Center for Energy Storage Research Argonne National LaboratoryLemontIL 60439USA Chemical Sciences and Engineering Division Argonne National LaboratoryLemontIL 60439USA

The performance of rechargeable batteries and other electrochemical systems depends on the rate at which the working ion(often a cation)is transported from one electrode to the other.The cation transference number is an important transport parameter that affects this rate.The purpose of this perspective is to distinguish between approximate and rigorous methods used in the literature to measure the transference number.We emphasize the fact that this parameter is dependent on the reference frame used in the analysis;care must be taken when comparing values obtained from different sources to account for differences in reference frames.We present data obtained from a well-characterized electrolyte.We compare rigorously determined transference numbers in two reference frames with values obtained by an approximate method.We conclude with a qualitative discussion of the relationship between the transference number and salt concentration gradients that are obtained when current is drawn through a battery。

关键词： battery electrolytes concentrated solution theory ion transport reference frames transference number

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Osmotic-Enhanced-Photoelectrochemical Hydrogen Production Based on Nanofluidics

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CCS Chemistry 2023年第9期5卷 2012-2022页

作者： Pei Liu Xiao-Ya Gao Li-Jun Zhang Weipeng Chen Yuhao Hu Xiang-Yu Kong Xu-Bing Li Liping Wen Chen-Ho Tung Li-Zhu Wu Lei Jiang Key Laboratory of Bio-inspired Materials and Interfacial Science Key Laboratory of Photochemical Conversion and Optoelectronic MaterialsTechnical Institute of Physics and ChemistryChinese Academy of SciencesBeijing 100190 School of Future Technology University of Chinese Academy of SciencesBeijing 100049

Harvesting clean energy such as solar energy and salinity gradient energy directly from the surrounding environment has attracted great attention.A promising proof-of-concept combination of cation-selective membrane-based osmotic energy with photoelectrochemical-based solar energy has been developed,highlighting the great potential for the direct conversion of osmotic energy to hydrogen energy.With the help of a 50-fold concentration gradient,the MXene-CdSe quantum dots system exhibits the highest photocurrent enhancement ratio(Δ/_(L-H)/Δ/_(L-L)),and the hydrogen production is increased by about 33%at a bias of 0 V versus reversible hydrogen electrode.Directly converting osmotic energy and solar energy into hydrogen energy suggests the possibility of coupling osmotic energy with other renewable energy sources.

关键词： nanofluidics ion transport H2 evolution energy conversion artificial photosynthesis

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An Anionic Covalent Organic Framework as an Electrostatic Molecular Rectifier for Stabilizing Mg Metal Electrodes

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CCS Chemistry 2023年第11期5卷 2567-2575页

作者： Zhongping Li Hyunseok Moon Seok-Kyu Cho Changqing Li Jeong-Min Seo Jong-Beom Baek Hong Xu Sang-Young Lee Department of Chemical and Biomolecular Engineering Yonsei UniversitySeoul 03772 School of Energy and Chemical Engineering Ulsan National Institute of Science and TechnologyUlsan 44919 UBATT Inc. Daejeon 34036 Institute of Nuclear and New Energy Technology Tsinghua UniversityBeijing 100084

Despite its potential as a high-capacity battery electrode,magnesium(Mg)metals are highly susceptible to electrolytes,resulting in the formation of unwanted passivation layers,which hinder charge transfer phenomena.Here,we first report an anionic covalent organic framework(a-COF)as an electrostatic molecular rectifier(that can preferentially trap solvent molecules)to stabilize Mg metal electrodes.Compared to a neutral COF(n-COF)as a control sample,the a-COF enhances Mg^(2+)transport by facilitating the desolvation of Mg^(2+)-solvent complexes and cationic mobility through its negatively charged one-dimensional columns,thereby achieving an ionic conductivity eight times higher than that of the n-COF.In addition,the anionic porous frameworks in contact with Mg metal electrodes enable a uniform Mg^(2+)flux and interfacial stability with Mg metal electrodes.Consequently,the a-COF exhibited reversible Mg plating/stripping cyclability on Mg metal electrodes compared to the n-COF,demonstrating the electrochemical viability of the anionic frameworks for Mg metal electrode stabilization.

关键词： anionic covalent organic framework Mg metal electrodes ion transport interfacial stability Mg plating/stripping

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Transcriptional profiles in zebrafish atp7a mutants and responses of atp7a mutants to Cu stress

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Water Biology and Security 2023年第3期2卷 87-97页

作者： You Wu Wenye Liu Lingya Li Zhipeng Tai Jing-Xia Liu College of Fisheries Key Laboratory of Freshwater Animal BreedingMinistry of AgricultureHuazhong Agricultural UniversityWuhan430070China

As a copper(Cu)transport ATPase,ATP7A plays an important role in maintaining Cu homeostasis in the body,but the developmental and physiological roles of atp7a in zebrafish embryogenesis are rarely studied.In this study,normal morphological phenotypes of atp7a^(−/−)homozygous zebrafish were observed at both embryonic and adult stages,however,atp7a^(−/−)larvae exhibited delayed touch response and obvious transcriptome changes.Compared with the WT(wild type),differentially expressed genes(DEGs)in atp7a^(−/−)larvae showed the enrichment in gene ontology(GO)terms related to several processes including ATPase activity,oxidoreductase activity,active transmembrane transporter activity,ion binding,and the citrate cycle.Furthermore,decreases in both ATP content and Na+/K+-ATPase activity in atp7a^(−/−)embryos and larvae were unveiled.57 overlapping DEGs were found both in WT stressed with Cu and in WT mutated with atp7a,and GO term analysis indicated the enrichment in the genes related to neurexin family protein binding and neuronal cell-cell adhesion.Moreover,42 overlapping DEGs in Cu stressed WT and Cu stressed atp7a^(−/−)were identified.GO term analysis showed an enrichment in the genes related to heme binding,implying that Cu was independent of the integral function of atp7a to affect heme binding.In addition,genes involved in the negative regulation of angiogenesis were down-regulated in atp7a^(−/−)mutants with and without Cu stress,which failed to occur in WT,implying that the integral function of atp7a is required for maintaining the normal expression of angiogenesis genes.The integrative data in this study demonstrated that atp7a is required for ion transport and angiogenesis,and for Cu-induced neurexin family protein binding defects,rather than for Cu-induced heme binding defects,during zebraﬁsh embryogenesis.These findings provide possible clues for human diseases with ATP7A dysfunction and imbalanced Cu homeostasis.

关键词： Angiogenesis ATP7A Cu stress Heme binding ion transport Neurexin family protein binding

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支柱策略增强离子传输和结构稳定性的KVPO4F用于超稳定的钾离子电池正极

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Science Bulletin 2023年第6期68卷 593-602,M0004页

作者：赵敬秦棪阳李龙吴虎贾鑫朱小龙赵洪洋苏亚琼丁书江 School of Chemistry University Engineering Research Center of Shaanxi ProvinceEngineering Research Center of Energy Storage Materials and Devices(Ministry of Education)Xi’an Jiaotong UniversityXi’an 710049China

近年来,由于丰富的钾资源储量和低廉的价格,钾离子电池在大规模储能领域表现出极大的应用前景.开发具有高安全性、高能量密度、低成本、长寿命的正极材料是推动钾离子电池实用化的关键.KVPO4F(KVPF)因其工作电压高、能量密度高、热稳定... 详细信息

近年来,由于丰富的钾资源储量和低廉的价格,钾离子电池在大规模储能领域表现出极大的应用前景.开发具有高安全性、高能量密度、低成本、长寿命的正极材料是推动钾离子电池实用化的关键.KVPO4F(KVPF)因其工作电压高、能量密度高、热稳定性好,被认为是一种很有前途的钾离子电池正极材料.然而,由于大半径的钾离子反复脱出/嵌入导致较慢的动力学和大的体积变化,从而影响材料循环稳定性.本文通过将大半径铯离子引入KVPF结构中的“支柱”策略,可有效提高材料的离子传导特性,并改善充放电过程中材料的结构稳定性,从而实现铯掺杂的KVPF正极优异的储钾性能.同时,高循环稳定性的KVPF//石墨全电池也展示了其在钾离子电池中巨大的实际应用潜力.

关键词： ion transport Structural stability KVPO4F Cs-substitution Stable potassium-ion batteries

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A High-Performance Solid-State Na–CO_(2)Battery with Poly(Vinylidene Fluoride-co-Hexafluoropropylene)−Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)Electrolyte

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Energy & Environmental Materials 2023年第3期6卷 87-95页

作者： Liang Lu Chunwen Sun Jian Hao Zelin Wang Sergio F.Mayer Maria Teresa Fernandez-Diıaz Jose Antonio Alonso Bingsuo Zou School of Chemical&Environmental Engineering China University of Mining and Technology-BeijingBeijing 100083China School of Physical Science and Technology Guangxi UniversityNanning 530004China State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering Ningxia UniversityYinchuan 750021China Instituto de Ciencia de los Materiales de Madrid CSICE-28049Cantoblanco-MadridSpain Institut Laue Langevin Grenoble F-38042France Guangxi Key Lab of Processing for Nonferrous Metals and Featured Materials and Key lab of new Processing Technology for Nonferrous Metals and Materials Ministry of EducationSchool of ResourcesEnvironments and MaterialsGuangxi UniversityNanning 530004China

The recovery and utilization of carbon dioxide(CO_(2))is the key to achieve the targets of peak carbon dioxide emissions and carbon neutrality.The Na-CO_(2)battery made with cheap alkali metal sodium and greenhouse gas CO_(2)is an effective strategy to consume CO_(2)and store clean renewable energy.However,the liquid electrolyte volatilization in the open battery system and inevitable dendrite growth restrict the application of Na-CO_(2)batteries.In this work,magnesium-doped Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)was studied as a solid electrolyte for solid-state Na-CO_(2)batteries.The ionic conductivity of Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)reaches 1.16 mS cm^(−1)at room temperature by replacing Zr ions in Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)with Mg ions,and the structural changes are analyzed by neutron powder diffraction.The composite electrolyte consisting of highly conductive Na_(3.2)Zr_(1.9)Mg_(0.1)Si_(2)PO_(12)and high processability poly(vinylidene fluoride-co-hexafluoropropylene)(PVDF-HFP)is utilized for the first time to assemble a solid-state Na-CO_(2)battery.The cell shows a full discharge capacity of 7720 mAh g^(−1)at 200 mA g^(−1).The middle gap voltage is lower than 2 V after 120 cycles at 200 mA g^(−1)and at a cut-off capacity of 500 mAh g^(−1).This work demonstrates a promising strategy to design high-performance solid-state Na-CO_(2)batteries.

关键词： cycling stability ion transport Mg-doped NZSP neutron powder diffraction solid-state Na-CO_(2)batteries

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One-step wet-spinning assembly of twisting-structured graphene/carbon nanotube fiber supercapacitor

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Journal of Energy Chemistry 2020年第12期29卷 434-441页

作者： Zhengpeng Yang Yuanheng Jia Yutao Niu Yongyi Zhang Chunjing Zhang Ping Li Meng Zhu Qingwen Li Henan Key Laboratory of Materials on Deep-Earth Engineering School of Materials Science and EngineeringHenan Polytechnic UniversityJiaozuo 454003HenanChina Key Laboratory of Multifunctional Nanomaterials and Smart Systems Advanced Materials DivisionSuzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of SciencesSuzhou 215123JiangsuChina School of Nano-Tech and Nano-Bionics University of Science and Technology of ChinaHefei 230026AnhuiChina Division of Nanomaterials and Jiangxi Key Lab of Carbonene Materials Suzhou Institute of Nano-Tech and Nano-BionicsNanchangChinese Academy of SciencesNanchang 330200JiangxiChina

Graphene fiber-based supercapacitors hold great promise as flexible energy-storage devices. However, simultaneously achieving high ion-transport ability in electrode and electrolyte layer, which is crucial for realizing the high electrochemical performance, still remains challenging. Here, a facile and effective strategy to solve the problem was proposed by developing a twisting-structured graphene/carbon nanotube(CNT) fiber supercapacitor via one-step wet-spinning process with customized multi-channel spinneret.The remarkable structure features of the resulting fiber supercapacitor with wrinkled and thin electrolyte layer, and well-developed porosity of fiber electrode favored the rapid infiltration and transport of electrolyte ions inside the electrode, as well as between electrode and electrolyte, thus boosting high specific capacitance of 187.6 mF cm^(-2) and energy density of 30.2 μWh cm^(-2), and featuring long cycling life(93%capacitance retention after 10,000 cycles) and excellent flexibility. Moreover, the specific capacitance and energy density could be further improved to 267.2 m F cm^(-2) and 66.8 μWh cm^(-2), respectively, when Mn O2 was incorporated into the fiber.

关键词： One-step wet-spinning Graphene fiber-based supercapacitor Twisting-structured fiber ion transport

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Real-time and in-situ intracellular ATP assay with polyimidazolium brush-modified nanopipette

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Science China Chemistry 2020年第7期63卷 1004-1011页

作者： Kailin Zhang Tianyi Xiong Fei Wu Qingwei Yue Wenliang Ji Ping Yu Lanqun Mao Beijing National Laboratory for Molecular Sciences Key Laboratory of Analytical Chemistry for Living BiosystemsInstitute of Chemistrythe Chinese Academy of Sciences(CAS)Beijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The level and dynamics of adenosine 5’-triphosphate(ATP) in single living cells are closely related to many kinds of important physiological and pathological processes. Herein, we report a nanosensor based on polyimidazolium brush(PimB)-modified nanopipette for intracellular ATP assay, which shows good selectivity, high spatiotemporal resolution and excellent stability.Both the specific supramolecular interaction between polyimidazolium and ATP, and the rationally tunable property of the ion transport at a confined nanopipette enable the selective assay of ATP even in complex intracellular environment. Moreover, the tiny tip(ca.300 nm) and the low polarized current(e.g., 1 nA) essentially make the as-prepared nanosensor safe to the living cells. The nanosensor is demonstrated to be useful for in-situ monitoring the basal ATP levels of chromaffin cells from wild-type mice and DJ-1 knockout mice, and for real-time monitoring the metabolism process of intracellular ATP.

关键词： intracellular ATP nanosensor ion transport single-cell analysis supramolecular interaction

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