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Modulated noble metal/2D MOF heterostructures for improved hydrogen storage of MgH2

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Rare Metals 2024年第4期43卷 1672-1685页

作者： Zeng-Yi Li Li-Xian Sun Fen Xu Yu-Mei Luo Yong-Peng Xia Sheng Wei Chen-Chen Zhang Ri-Guang Cheng Chao-Feng Ye Meng-Yuan Liu Ju-Lan Zeng Zhong Cao Hong-Ge Pan School of material science and Engineering Guilin University of Electronic Technology School of Chemistry and Chemical Engineering Changsha University of Science and Technology institute of science and Technology for New energy Xi'an Technological University

The conjugation of external species with twodimensional（2D） materials has broad application prospects.In this study,we have explored the potential of noble metal/2D MOF heterostructures in hydrogen storage.Specifically,the MgH2-Ni-MOF@Pd system has shown remarkable hydrogen desorption/sorption performances,starting to liberate hydrogen at 181 0C,which is 230 0C lower than that of pristine MgH2.Under the catalytic effect of Ni-MOF@Pd,the dehydrogenation apparent activation energy of MgH2 is noticeably decreased from（133.5 ± 17.5） to（34.58 ± 1.87） kJ·mol-1,and the hydrogenation apparent activation energy is reduced from（70.41 ± 7.43） to（25.78 ± 4.64） kJ·mol-1,which is lowered by 63.4%.The fully-dehydrogenated MgH2-NiMOF@Pd composite rapidly uptakes hydrogen,with 2.62wt% at 100℃ and 6.06 wt% at 150℃ within 300 s,respectively.The mechanism analysis of MgH2 catalyzed by Ni-MOF@Pd has revealed that the transformation of Mg2Ni and Mg2NiH4could act as a "hydrogen pump",providing numerous channels for fast diffusion and transport of hydrogen atoms.Moreover,in the dehydrogenation process,the element Pd reacts with MgH2to form the MgPd alloy phase,which makes MgH2take precedence to decompose through the Mg-Pd alloy rather than self-decomposition,further reducing thermal stability and improving de/hydrogenation kinetics.The synergistic effect of Mg-Pd,Mg2Ni,and the special ultra-thin 2D sheet structure of the additive is the main reason for the good hydrogen storage property of MgH2-Ni-MOF@Pd.Our findings provide inspiration for designing efficient multifunctional additives with unique morphologies to optimize the hydrogen desorption/sorption behaviors of hydrogen storage materials.

关键词： Hydrogen storage Magnesium hydride 2D metal-organic framework nanosheets Ni/Pd Synergistic catalysis

Recent Progress in All-Solution-Processed Organic Solar Cells

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Chinese Journal of Chemistry 2024年第2期42卷 190-198页

作者： Yixuan Xu Qian Wang Wentao Zou Xu Zhang Yanna Sun Yuanyuan Kan Ping Cai Ke Gao School of materials science and Engineering&Guangxi Key Laboratory of Information materials Guilin University of Electronic TechnologyGuilinGuangxi 541004China Shandong Provincial Key Laboratory for science of material Creation and energy Conversion Science Center for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong UniversityQingdaoShandong 266237China

All-solution-processed organic solar cells(OSCs)(from the bottom electrode to the top electrode)are highly attractive thanks to their low cost,lightweight and high-throughput production.However,achieving highly efficient all-solution-processed OSCs remains a significant challenge.One of the key issues is the lack of high-quality solution-processed electrode systems that can replace indium tin oxide(ITO)and vacuum-deposited metal electrodes.In this paper,we comprehensively review recent advances in all-solution-processed osCs,and classified the devices as the top electrode materials,including silver nanowires(AgNWs),conducting polymers and composite conducting materials.The correlation between electrode materials,properties of electrodes,and device performance in all-solution-processed OSCs is elucidated.In addition,the critical roles of the active layer and interface layer are also discussed.Finally,the prospects and challenges of all-solution-processed OSCs are presented.

关键词： Organic solar cells All-solution-processed organic solar cells Solution-processed electrodes High performance Silver nanowires Conductive polymers Composite conducting materials

Lithiated Graphdiyne Quantum Dots for Stable Lithium Metal Anodes

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CCS Chemistry 2024年第5期6卷 1300-1311页

作者： Han Shen Congying Song Fan Wang Guoxing Li Yuliang Li Shandong Provincial Key Laboratory for science of material Creation and energy Conversion Science Center for Material Creation and Energy ConversionInstitute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237 Key Laboratory of Organic Solids Institute of ChemistryChinese Academy of SciencesBeijing 100190 University of Chinese Academy of sciences Beijing 100049

Here,a facile strategy is proposed for the preparation of lithiated graphdiyne quantum dots(GDY-Li QDs)with conjugated sp-and sp2-hybridized carbons by the self-assembly technique ofπ–πstacking of lithiated hexaethynylbezene under mild conditions.The as-prepared GDY-Li QDs,containing stacked multialkynyl aromatic backbone and abundant lithium(Li),show an average diameter of about 2.6 nm and good dispersion in the solvents.These distinctive structures endow GDY-Li QDs with superior properties that cannot be matched by traditional QDs,such as strong ion adsorption,Li-ion self-concentration,high Li-ion conductivity,the nanoconfinement effect,and ion solvation regulation.Benefiting from these features,GDY-Li QDs can stabilize Limetal anodes to effectively suppress Li-dendrite growth and significantly improve its Li plating/stripping coulombic efficiency(99.3%in the carbonate electrolyte).The full cells with GDY-Li QDs protected Li-metal anodes,and LiNi0.8Co0.1Mn0.^(1)O_(2)cathodes delivered high capacity and excellent cycling stability at high rates,which demonstrates the great potential of GDY-Li QDs for application in fast-charging Li-metal batteries.

关键词： graphdiyne quantum dots lithiation lithium metal anodes ion distribution

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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Enhanced activity and durability of FeCoCrMoCBY nanoglass in acidic hydrogen evolution reaction

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Journal of materials science & Technology 2024年第3期170卷 212-220页

作者： Mengyang Yan Shuangqin Chen Shangshu Wu Xuechun Zhou Shu Fu Di Wang Christian Kübel Horst Hahn Si Lan Tao Feng Herbert Gleiter institute of Nanoscience School of Material Science and EngineeringNanjing University of Science and TechnologyNanjing 210094China institute of Nanotechnology Karlsruhe Institute of TechnologyKarlsruhe 76021Germany

In the present work,a multi-element nanoglass(m-NG)of FeCoCrMoCBY is obtained first time by the laser ablation combined with inert gas condensation(laser-IGC)technique.Compared with the conventional rapid-quenched metallic glass(MG)with identical composition,the Fe-based m-NG demonstrates a superior performance as a self-supported electrocatalyst for hydrogen evolution reaction(HER)in acidic solution.The enhanced HER activity of m-NG is proposed to be closely related to its high en-ergy states,which is originated from the unique inhomogeneous nanostructures with a high density of low-coordinated atoms.Additionally,the Fe-based m-NG exhibits an outstanding comprehensive catalytic performance even beyond the commercial Pt/C catalyst in long-term test due to its self-optimization ability.This work not only opens the way to the preparation of m-NGs by the novel laser-IGC technique,but also makes a great contribution to developing low-cost,high-efficient,and super-durable HER electrocat-alysts in acidic environment.

关键词： Nanoglass Inert gas condensations High energy states Hydrogen evolution reactions

Sensitizing photoactive metal-organic frameworks via chromophore for significantly boosting photosynthesis

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Chinese Chemical Letters 2024年第5期35卷 519-522页

作者： Lihua Ma Song Guo Zhi-Ming Zhang Jin-Zhong Wang Tong-Bu Lu Xian-Shun Zeng School of materials science and Engineering Harbin Institute of TechnologyHarbin 150001China institute for New energy materials and Low Carbon Technologies School of Material Science&EngineeringTianjin University of TechnologyTianjin 300384China

Photosensitization related to energy/electron transfer process is of great importance to natural photosynthesis.Herein,we proposed a promising strategy to improve the sensitizing ability of the typical photoactive MOFs(UiO-Ir)by engineering its metal coordination center with NBI(1,8-naphthalenebenzimidizole)chromophore.The resulting MOFs(UiO-Ir-NBI)exhibited a strong sensitizing ability for significantly boosting photosynthesis.Impressively,the catalytic yield of 2-chloroethyl ethyl sulfoxide with UiO-Ir-NBI can reach 99%,over 6 times higher than that with UiO-Ir(16.4%).Moreover,UiO-Ir-NBI exhibited an excellent catalytic stability and a broad substrate tolerance,highlighting its great application prospect.Systematic investigations revealed that the strong visible light absorption,long excited state lifetime and efficient electron-hole separation of UiO-Ir-NBI greatly contributed to harvesting visible light and facilitating interface electron/energy transfer for efficient solar energy utilization.This work provides a new horizon to boost photosythesis of MOFs by engineering their metal sensitizing centers at a molecular level.

关键词： Metal-organic framework Photocatalysis Excited state Strong visible absorption Iridium complex

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Achieving high-efficient photocatalytic persulfate-activated degradation of tetracycline via carbon dots modified MIL-101(Fe)octahedrons

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Chinese Journal of Chemical Engineering 2024年第2期66卷 298-309页

作者： Hao Yuan Xinhai Sun Shuai Zhang Weilong Shi Feng Guo School of material science and Engineering Jiangsu University of Science and TechnologyZhenjiang 212003China School of energy and Power Jiangsu University of Science and TechnologyZhenjiang 212003China

The synergistic reaction of photocatalysis and advanced oxidation is a valid strategy for the degradation of harmful antibiotic wastewater.Herein,carbon dots(CDs)modified MIL-101(Fe)octahedrons to form CDs/MIL-101(Fe)composite photocatalyst was synthesized for visible light-driven photocatalytic/persulfate(PS)-activated tetracycline(TC)degradation.The electron spin resonance(ESR)spectra,scavenging experiment and electrochemical analysis were carried out to reveal that the high visible light-driven photocatalytic degradation activity of TC over CDs/MIL-101(Fe)photocatalysts is not only ascribed to the production of free active radicals in the CDs/MIL-101(Fe)/PS system(·OH,·SO_(4-),^(1)O_(2),h^(+)and·O_(2)^(-))but also attributed to the consumption of electrons caused by the PS,which can suppress the recombination of photo-generated carriers as well as strong light scattering and electron trapping effects of CDs.Finally,the possible degradation pathways were proposed by analyzing intermediates via liquid chromatography-mass spectrometry technique.This research presents a rational design conception to construct a CDs/PS-based photocatalysis/advanced oxidation technology with high-efficient degradation activity for the remediation of organic antibiotic pollutant wastewater and for the improvement of carrier transport kinetics of photocatalysts.

关键词： Carbon dots MIL-101(Fe) Photocatalytic Persulfate activation Tetracycline degradation

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An Ion-Pumping Interphase on Graphdiyne/Graphite Heterojunction for Fast-Charging Lithium-Ion Batteries

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CCS Chemistry 2024年第1期6卷 110-124页

作者： Juan An Fan Wang Jia-Yue Yang Guoxing Li Yuliang Li Shandong Provincial Key Laboratory for science of material Creation and energy Conversion Science Center for Material Creation and Energy ConversionSchool of Chemistry and Chemical EngineeringInstitute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237 Optics&Thermal Radiation Research Center Institute of Frontier and Interdisciplinary ScienceShandong UniversityQingdao 266237 institute of Chemistry The Chinese Academy of SciencesBeijing 100190 University of Chinese Academy of sciences Beijing 100049

The sluggish lithium-ion(Li-ion)transport kinetics in graphite anode hinders its application in fast-charging Li-ion batteries(LIBs).Here,we develop an ionpumping interphase(IPI)on graphdiyne(GDY)/graphite heterojunction anodes to boost the ionic transport kinetics and enable high-performance,fast-charging LIBs.The IPI changed the ion solvation/desolvation environment by covalent/non-covalent interactions with Li ions or solvents to optimize solid-electrolyte interphase(SEI)and regulate Li-ion transport behavior.We studied the in situ growth of few-layer GDY on graphite surface(GDY/graphite)as the IPI and found that the strong interaction between GDY and Li ions enabled surface-induced modification of the ion solvation behavior and surface-assisted desolvation effect to accelerate the Li-ion desolvation process.A functional anion-derived SEI layer with improved Li-ion conductivity was created.Together with the generated built-in electric field at GDY/graphite hetero-interface self-pumping Li ions to intercalate into the graphite,the Li-ion transport kinetics was significantly enhanced to effectively eliminate Li plating and large voltage polarization of the graphite anodes.A fast Li intercalation in GDY/graphite without Li oversaturation at the edge of the graphite was directly observed.The superior performance with high capacity(139.2 mA h g^(-1))and long lifespan(1650 cycles)under extremely fast-charging conditions(20 C,1 C=372 mA g^(-1))was achieved on GDY/graphite anodes.Even at low temperatures(-20℃),a specific capacity of 128.4 mA h g^(-1) was achieved with a capacity retention of 80%after 500 cycles at a 2 C rate.

关键词： extreme fast-charging lithium-ion batteries lithium-ion transport kinetics ion-pumping interphase graphdiyne/graphite heterojunction

Manipulating fast Li_(2)S redox via carbon confinement and oxygen defect engineering of In_(2)O_(3)for lithium-sulfur batteries

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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