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The dynamic surface evolution of halide perovskites induced by external energy stimulation

National Science Review 2024年第4期11卷 185-194页

作者： Feiyu Cheng Pengdong Wang Chenzhe Xu Qingliang Liao Suicai Zhang Haochun Sun Wenqiang Fan Guodong Liu Zhiyun Li Yaping Kong Li Wang Fangsen Li Zhuo Kang Yue Zhang Academy for Advanced Interdisciplinary Science and Technology State Key Laboratory for Advanced Metals and Materials University of Science and Technology Beijing Beijing Key Laboratory for Advanced Energy materials and Technologies Key Laboratory of Advanced Materials and Devices for Post-Moore ChipsMinistry of EducationBeijing Advanced Innovation Center for Materials Genome Engineering School of Materials Science and EngineeringUniversity of Science and Technology Beijing Vacuum Interconnected nanotech Workstation(nano-X) Suzhou Institute of Nano-Tech and Nano-BionicsChinese Academy of Sciences Beijing National Laboratory for Condensed Matter Physics Institute of Physics Chinese Academy of Sciences

Tracking the dynamic surface evolution of metal halide perovskite is crucial for understanding the corresponding fundamental principles of photoelectric properties and intrinsic instability. However, due to the volatility elements and soft lattice nature of perovskites, several important dynamic behaviors remain unclear. Here, an ultra-high vacuum（UHV） interconnection system integrated by surface-sensitive probing techniques has been developed to investigate the freshly cleaved surface of CH3NH3PbBr3in situ under given energy stimulation. On this basis, the detailed three-step chemical decomposition pathway of perovskites has been clarified. Meanwhile, the evolution of crystal structure from cubic phase to tetragonal phase on the perovskite surface has been revealed under energy stimulation. Accompanied by chemical composition and crystal structure evolution, electronic structure changes including energy level position,hole effective mass, and Rashba splitting have also been accurately determined. These findings provide a clear perspective on the physical origin of optoelectronic properties and the decomposition mechanism of perovskites.

关键词： metal halide perovskite external energy stimulation surface dynamic evolution surface electronic structure ultra-high vacuum interconnection system

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Cage-confinement synthesis of MoC nanoclusers as efficient sulfiphilic and lithiophilic regulator for superior Li–S batteries

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Rare Metals 2024年第2期43卷 624-634页

作者： Xing-Yuan Zhang Mei-Na Lei Shan Tian Jian-Gan Wang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Laboratory of Graphene(NPU)Xi’an710072China

High-energy-density Li-S batteries are subjected to serious sulfur deactivation and short cycle lifetime caused by undesirable polysulfide shuttle effect and frantic lithium dendrite formation.In this work,a controllable cage-confinement strategy to fabricate molybdenum carbide(MoC)nanoclusters as a high-efficient sulfiphilic and lithiophilic regulator to mitigate the formidable issues of Li-S batteries is demonstrated.The sub-2 nm MoC nanoclusters not only guarantee robust chemisorption and fast electrocatalytic conversion of polysulfides to enhance the sulfur electrochemistry,but also homogenize Li^(+) flux to suppress the lithium dendrite growth.As a consequence,the MoC-modified separator endows the batteries with boosted reaction kinetics,promoted sulfur utilization,and improved cycling stability.A reversible capacity of 701 mAh·g^(−1) at a high rate of 5.0C and a small decay rate of 0.076%per cycle at 1.0C over 600 cycles are achieved.This study offers a rational route for design and synthesis of bifunctional nanoclusers with both sulfiphilicity and lithiophilicity for high-performance Li-S batteries.

关键词： Li-S batteries nanocluster Electrocatalyst Polysulfide shuttle Li dendrites

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Complementary multicolor electrochromic devices with excellent stability based on porous tin oxide nanosheet scaffold

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nano Research 2024年第4期17卷 3035-3042页

作者： Chenchen Bian Jinhui Wang Huanhuan Liu Yin Yan Ping Zhang Weilong Yang Sensen Jia Xiaodan Guo Guofa Cai Key Laboratory for Special Functional materials of Ministry of Education National&Local Joint Engineering Research Center for High-Efficiency Display and Lighting TechnologySchool of Materials and Engineeringand Collaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityKaifeng 475004China

Electrochromic devices(ECDs)have been extensively investigated as promising candidates in broad cutting-edge applications,such as smart windows,electronic labels,adaptive camouflage,etc.However,they have suffered from either inadequate color variations or poor cycling stability for a long time.Herein,we developed a general strategy to boost the cyclic stability and enrich the color variations of ECDs by scrupulous design of the composition and nanostructure of electrodes,in which porous tin oxide(SnO_(2))nanosheets serve as the scaffold and typical metal oxides or conducting polymers as the active electrochromic materials.Various electrochromic composite materials,including polyaniline(PANI)@SnO_(2),V2O5@SnO_(2),and WO_(3)@SnO_(2) heterostructured nanoarrays were prepared by the facile wet-chemical method.These composite electrodes exhibit remarkable electrochromic performances,e.g.,superior cycling stability(more than 2000 cycles),rich color variations(more than 5 colors for PANI@SnO_(2)),and enlarged optical modulation.These excellent performances account for the heterogenous porous nanoarrays,which not only facilitate the intercalation/extraction of ions but also relieve the stress generated during the electrochemical process.In addition,diverse prototypes of complementary multicolor ECD with excellent cycling stability(over thousands of cycles)and rich color variations(8 colors)were realized for the first time.We believe that our work put forward a general strategy for developing high-quality multicolor complementary electrochromic devices.

关键词： electrochromism tin oxide metal oxide cycling stability multicolor complementary device

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Regulation of pseudographitic carbon domain to boost sodium energy storage

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nano Research 2024年第6期17卷 5188-5196页

作者： Zhidong Hou Mingwei Jiang Da Lei Xiang Zhang Yuyang Gao Jian-Gan Wang State Key Laboratory of Solidification Processing Center for Nano Energy MaterialsSchool of Materials Science and EngineeringNorthwestern Polytechnical University and Shaanxi Joint Lab of Graphene(NPU)Xi’an 710072China

Hard carbon anode has shown extraordinary potentials for sodium-ion batteries(SIBs)owing to the cost-effectiveness and advantaged microstructure.Nevertheless,the widespread application of hard carbon is still hindered by the insufficient sodium storage capacity and depressed rate property,which are mainly induced by the undesirable pseudographitic structure.Herein,we develop a molten-salt-mediated strategy to regulate the pseudographitic structure of hard carbon with suitable interlayer spacing and enlarged pseudographitic domain,which is conducive to the intercalation capacity and diffusion kinetics of sodium ions.Impressively,the optimized hard carbon anode delivers a high reversible capacity of 320 mAh·g^(−1),along with superior rate property(138 mAh·g−1 at 2 A·g^(−1))and stable cyclability over 1800 cycles.Moreover,the in situ Raman spectroscopic study and full-cell assembly further investigate the sodium storage mechanism and practical implement of obtained hard carbon.This work pioneers a low-cost and effective route to regulate the pseudographitic structure of hard carbon materials for advanced SIBs.

关键词： pseudographitic structure molten salt hard carbon anode sodium-ion batteries

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Graphene from microwave-initiated upcycling of waste polyethylene for electrocatalytic reduction of chloramphenicol

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Chinese Chemical Letters 2024年第4期35卷 187-192页

作者： Qiang Cao Xue-Feng Cheng Jia Wang Chang Zhou Liu-Jun Yang Guan Wang Dong-Yun Chen Jing-Hui He Jian-Mei Lu College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhou 215123China

Waste polyolefin plastics, accounting for 50% of all plastic waste, represent a tremendously unexploited carbon source. Efficiently upcycling polyolefin waste into value-added carbon materials for waste water treatment avoiding using noble metals is challenging but economically and environmentally sustainable. In this work, MAX-Ti_(3)AlC_(2) supported Fe selectively catalyzes polyolefin into few-layered graphene in 5 min under microwave treatment. Graphene and MAX supported Fe(Fe@MLC) can completely(99.9%)degrade chloramphenicol(CAP) within 60 min, retain robust after 10 cycles and work efficiently at a wide p H range(3.87–13.03), avoiding the usage of noble metal. Moreover, the electrochemical active surface area(ECSA) of Fe@MLC is 2.7 times higher than that of commercial Pt/C. This work provides a cheap and efficient catalyst that promotes deconstruction of plastic wastes and indirectly degrades antibiotics thereby realizes the treatment of waste water with waste plastic.

关键词： Microwave Ti_(3)AlC_(2) Electrochemistry Dechlorination Chloramphenicol

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Regulation of the quantum barrier and carrier transport toward high-efficiency quasi-2D Dion-Jacobson tin perovskite solar cells

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Journal of Energy Chemistry 2024年第8期95卷 200-207页

作者： Huanhuan Yao Chang Shi Tai Wu Shurong Wang Mingyu Yin Liming Ding Yong Hua Feng Hao School of materials and Energy University of Electronic Science and Technology of China College of Chemistry and Molecular Engineering Peking University Yunnan Key Laboratory for Micro/nano materials & Technology School of Materials and Energy Yunnan University center for Excellence in nanoscience (CAS) Key Laboratory of Nanosystem and Hierarchical Fabrication (CAS) National Center for Nanoscience and Technology

Quasi-2D Dion-Jacobson（DJ） tin halide perovskite has attracted much attention due to its elimination of Van der Waals gap and enhanced environmental stability.However,the bulky organic spacers usually form a natural quantum well structure,which brings a large quantum barrier and poor film quality,further limiting the carrier transport and device performance.Here,we designed three organic spacers with different chain lengths(ethylenediamine（EDA）,1,3-propanediamine（PDA）,and 1,4-butanediamine（BDA）) to investigate the quantum barrier dependence.Theoretical and experimental characterizations indicate that EDA with short chain can reduce the lattice distortion and dielectric confinement effect,which is beneficial to the effective dissociation of excitons and the inhibition of trap-free non-radiative relaxation.In addition,EDA cation shows strong interaction with the inorganic octahedron,realizing large aggregates in precursor solution and high-quality films with improved structural stability.Furthermore,femtosecond transient absorption proves that EDA cations can also weaken the formation of small n-phases with large quantum barrier to achieve effective carrier transport between different nphases.Finally,the quasi-2D DJ（EDA）FA9Sn10I31solar cells achieves a 7.07% power conversion efficiency with good environment stability.Therefore,this work sheds light on the regulation of the quantum barrier and carrier transport through the chain length of organic spacer for qua si-2D DJ lead-free perovskites.

关键词： Carrier transport Chain lengths Lattice distortion Organic spacers Quantum well

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Converting intercalation-type cathode in spent lithium-ion batteries into conversion-type cathode

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nano Research 2024年第5期17卷 4602-4609页

作者： Dingding Zhu Yong Su Jingzhao Chen Xiangze Ou Xuedong Zhang Wen Xie Yuyan Zhou Yunna Guo Qiushi Dai Peng Jia Jitong Yan Lin Geng Baiyu Guo Liqiang Zhang Yongfu Tang Qiao Huang Jianyu Huang School of materials Science and Engineering Xiangtan UniversityXiangtan 411105China Clean nano Energy center State Key Laboratory of Metastable Materials Science and TechnologyYanshan UniversityQinhuangdao 066000China

The widespread applications of lithium-ion batteries(LIBs)generate tons of spent LIBs.Therefore,recycling LIBs is of paramount importance in protecting the environment and saving the resources.Current commercialized LIBs mostly adopt layered oxides such as LiCoO_(2)(LCO)or LiNi_(x)Co_(y)Mn_(1-x-y)O_(2)(NMC)as the cathode materials.Converting the intercalation-type spent oxides into conversion-type cathodes(such as metal fluorides(MFs))offers a valid recycling strategy and provides substantially improved energy densities for LIBs.Herein,two typical Co-based cathodes,LCO and LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NMC622),in spent LIBs were successfully converted to CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) cathodes by a reduction and fluorination technique.The as converted CoF_(2) and(Ni_(x)Co_(y)Mn_(z))F_(2) delivered cell energy densities of 650 and 700 Wh/kg,respectively.Advanced atomic-level electron microscopy revealed that the used LCO and NMC622 were converted to highly phase pure Co metal and Ni_(0.6)Co_(0.2)Mn_(0.2) alloys in the used graphite-assisted reduction roasting,simultaneously producing the important product of Li_(2)CO_(3) using only environment friendly solvent.Our study provided a versatile strategy to convert the intercalation-type Co-based cathode in the spent LIBs into conversion-type MFs cathodes,which offers a new avenue to recycle the spent LIBs and substantially increase the energy densities of next generation LIBs.

关键词： spent lithium-ion batteries recycling energy densities conversion-type cathode

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Conceptual transition from molecular to atomic: unleashing a new era in hydrogen therapy for chronic disease

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National Science Review 2024年第4期11卷 17-18页

作者： Zhigang Zou Eco-materials and Renewable Energy Research center (ERERC) Jiangsu Key Laboratory for Nano Technology National Laboratory of Solid State Microstructures and Department of PhysicsNanjing University

The dysregulated overexpression of reactive oxygen and nitrogen species (RONS)intricately links to the occurrence and development of diverse chronic diseases[1–3]. Hydrogen therapy stands out as a promising treatment methodology recognized for effectively mitigating RONS and maintaining intracellular redox equilibrium, thereby yielding therapeutic benefits [4,5].

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Superwettable interface towards biodetection in confined space

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nano Research 2024年第2期17卷 602-617页

作者： Zexu Pang Zhikang Cao Wanlu Li Wenxia Xu Yingying Zhang Qitao Zhou Jing Pan Fan Xia State Key Laboratory of Biogeology and Environmental Geology Engineering Research Center of Nano-Geomaterials of the Ministry of EducationFaculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430074China

The detection of biomarkers with both high sensitivity and specificity is crucial for the diagnosis and treatment of related diseases.However,many current detections employ ex-situ detection method and non-confined condition,thus have many problems,which may eventually lead to inaccurate detection results.Compared to detection in non-confined space,detection in confined space can better reflect the real in-vivo situation.Therefore,the construction of detection for target molecules in confined space has great significance for both theoretical research and practical application.To realize the detection of target molecules in confined space,the probes should accurately enter the confined space where the target molecules reside and interact with the interface.Thus,how to explore and utilize the properties of the interface(for example,bioinspired superwettability)has always been a hot and difficult topic in this field.Herein,the recent advances and our efforts in recent 10 years on detection of bio-target molecules in confined space with superwettable interface have been introduced from the perspective of the detection methods.The suitable and most widely employed detection methods for target molecules in confined spaces are introduced firstly.Then,recent progresses for related detections based on visual,optical,and electrochemical detection methods are presented successively.Finally,the perspective for detection in confined space is discussed for the future development of biochemical detection.

关键词： biodetection superwettability confined space interface

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Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity

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nano Research 2024年第3期17卷 1232-1241页

作者： Yu Lin Defang Ding Shicheng Zhu Qunlei Wen Huangjingwei Li Zhen Li Youwen Liu Yi Shen China Engineering Research center of nano-Geomaterials of Ministry of Education Faculty of Materials Science and ChemistryChina University of GeosciencesWuhan 430078China State Key Laboratory of materials Processing and Die&Mould Technology and School of Materials Science and EngineeringHuazhong University of Science and TechnologyWuhan 430074China

Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic viability.Herein,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process.The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites.Furthermore,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni sites.By the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.

关键词： hydrogen evolution activity complementary multisite catalysts sequential reactive water management interfacial water molecules

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