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Highly selective and eco-friendly dihydroisoquinoline synthesis via Cu/Co synergistic catalysis in Cu NPs@MOFs catalyst under mild conditions

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Science China Chemistry 2024年第5期67卷 1561-1568页

作者： Peng-Fei Guo Ze-Long Liang Yue-E Jiao Hang Xu Bin Zhao Key Laboratory of Advanced energy Material Chemistry Renewable Energy Conversion and Storage CenterDepartment of ChemistryNankai UniversityTianjin 300071China

3,4-Dihydroisoquinoline(DHIQ)is an important precursor used in the production of drugs for treating cancer,HIV,Alzheimer's disease,*** studies on DHIQ synthesis show low catalytic selectivity due to the susceptible over-oxidation feedstock of1,2,3,4-tetrahydroisoquinoline(THIQ),which often requires alkali ***,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction ***,a novel framework 1 was synthesized,exhibiting 1D channels with the size of 4.6 A×9.6 A and high solvent/p H/thermal stability.A stable framework allows it to encapsulate Cu nanoparticles(NPs)to form Cu NPs@1-x(x=1,2,3,and 4)with varying loading amounts of Cu NPs at 2.0 wt%,3.0 wt%,4.0 wt%,and 6.0 wt%,*** NPs@1-3 could selectively catalyze the reaction from THIQ to DHIQ with a high selectivity of 98%and a recorded turnover frequency(TOF)of 22.1 h-1under eco-friendly mild *** corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale ***,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air ***,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@*** investigations revealed that high catalytic performance can be attributed to the stable framework and the synergistic catalytic effect of the loaded Cu NPs and Co metal *** importantly,this work represents the first example of MOF catalysts for selectively thermo-catalytic DHIQ synthesis and demonstrates a simple approach to obtain efficient catalysts for selective oxydehydrogenation in the production of unsaturated compounds.

关键词： metal-organic frameworks Cu NPs@MOFs 3 4-dihydroisoquinoline selective oxydehydrogenation synergistic catalysis

Visual and portable detection of metronidazole realized by metal-organic framework flexible sensor and smartphone scanning

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Chinese Chemical Letters 2024年第10期35卷 526-530页

作者： Xiangshuai Li Jian Zhao Li Luo Zhuohao Jiao Ying Shi Shengli Hou Bin Zhao Department of Chemistry Key Laboratory of Advanced Energy Materials Chemistry Renewable Energy Conversion and Storage Center (RECAST) Nankai University

Metronidazole （MNZ） is a type of antibiotic that can help people and animals cure bacterial in fections,however,abuse of MNZ has posed a threat to human ***,portable and vi sual detection of MNZ is meaningful for food safety and rational administration of drugs,bu full of ***,a porous three-dimensional Tb-based metal-organic framework (MOF{（CH3）2NH2·[Tb5（TDA）8（H2O）2]·6DMF·2C2H5OH}_n（TDA-Tb） with good solvent and p H stabilities was pre pared,and the framework possesses one-dimensional channels with a diameter of 12 A along the c-axis Experiment results suggest that the synthesized TDA-Tb can selectively and sensitively detect MNZ in water,and the limit of detection （LOD） is as low as 4.1×10-7mol/***,a flexible sensor TDA Tb-M was also constructed by incorporating TDA-Tb into membrane materials for convenient *** the TDA-Tb-M firstly realized portable and visual detection of MNZ through smartphone scanning,which may inspire more probes with wide application ranges.

关键词： Antibiotic Lanthanide Luminescence Metal-organic framework Sensor

An active learning workflow for predicting hydrogen atom adsorption energies on binary oxides based on local electronic transfer features

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Green energy & Environment 2024年第10期9卷 1489-1496页

作者： Wenhao Jing Zihao Jiao Mengmeng Song Ya Liu Liejin Guo International Research center for renewable energy State Key Laboratory of Multiphase Flow in Power Engineering Xi'an Jiaotong University Department of energy and Power Engineering Shandong University of Technology

Machine learning combined with density functional theory（DFT） enables rapid exploration of catalyst descriptors space such as adsorption energy, facilitating rapid and effective catalyst screening. However, there is still a lack of models for predicting adsorption energies on oxides,due to the complexity of elemental species and the ambiguous coordination environment. This work proposes an active learning workflow（Le NN） founded on local electronic transfer features（e） and the principle of coordinate rotation invariance. By accurately characterizing the electron transfer to adsorption site atoms and their surrounding geometric structures, Le NN mitigates abrupt feature changes due to different element types and clarifies coordination environments. As a result, it enables the prediction of *H adsorption energy on binary oxide surfaces with a mean absolute error（MAE） below 0.18 e V. Moreover, we incorporate local coverage（θl） and leverage neutral network ensemble to establish an active learning workflow, attaining a prediction MAE below 0.2 e V for 5419 multi-*H adsorption structures. These findings validate the universality and capability of the proposed features in predicting *H adsorption energy on binary oxide surfaces.

关键词： Machine learning Adsorption energy Binary oxide Electron transfer Active learning

Solar fuel production through concentrating light irradiation

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Green energy & Environment 2024年第10期9卷 1550-1580页

作者： Yiwei Fu Yi Wang Jie Huang Kejian Lu Maochang Liu International Research center for renewable energy State Key Laboratory of Multiphase Flow Xi'an Jiaotong University Suzhou Academy of Xi'an Jiaotong University

The climate crisis necessitates the development of non-fossil energy sources. Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure. However, solar fuel production is in its early stages of development, constrained by low conversion efficiency and challenges in scaling up production. Concentrated solar energy(CSE) technology has matured alongside the rapid growth of solar thermal power plants. This review provides an overview of current CSE methods and solar fuel production, analyzes their integration compatibility, and delves into the theoretical mechanisms by which CSE impacts solar energy conversion efficiency and product selectivity in the context of photo-electrochemistry, thermochemistry, and photo-thermal co-catalysis for solar fuel production. The review also summarizes approaches to studying the photoelectric and photothermal effects of CSE. Lastly, it explores emerging novel CSE technology methods in the field of solar fuel production.

关键词： Concentrated solar energy Solar fuel Photo-electrochemistry Thermochemistry Photo-thermal co-catalysis

Cascade utilization of full spectrum solar energy for achieving simultaneous hydrogen production and all-day thermoelectric conversion

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Journal of energy Chemistry 2024年第9期96卷 318-327页

作者： Tuo Zhang Liang Dong Baoyuan Wang Jingkuo Qu Xiaoyuan Ye Wengao Zeng Ze Gao Bin Zhu Ziying Zhang Xiangjiu Guan Liejin Guo International Research center for renewable energy(IRCRE) State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

Solar-driven photocatalytic water/seawater splitting holds great potential for green hydrogen ***,the practical application is hindered by the relatively low conversion efficiency resulting from the inadequate utilization of solar spectrum with significant waste in the form of ***,current equipment struggles to maintain all-day operation subjected to the lack of light during ***,a novel hybrid system integrating photothermal catalytic(PTC)reactor,thermoelectric generator(TEG),and phase change materials(PCM)was proposed and designed(named as PTC-TEG-PCM)to address these challenges and enable simultaneous overall seawater splitting and 24-hour power *** PTC system effectively maintains in an optimal temperature range to maximize photothermal-assisted photocatalytic hydrogen *** TEG component recycles the low-grade waste heat for power generation,complementing the shortcoming of photocatalytic conversion and achieving cascade utilization of full-spectrum solar ***,exceptional thermal storage capability of PCM allow for the conversion of released heat into electricity during nighttime,contributing significantly to the overall power output and enabling PTC-TEG-PCM to operate for more than 12 h under the actual *** to traditional PTC system,the overall energy conversion efficiency of the PTC-TEG-PCM system can be increased by∼500%,while maintaining the solar-to-hydrogen *** advancement of this novel system demonstrated that recycling waste heat from the PTC system and utilizing heat absorption/release capability of PCM for thermoelectric application are effective strategies to improve solar energy *** flexible parameter designing,PTC-TEG-PCM can be applied in various scenarios,offering high efficiency,stability,and sustainability.

关键词： Hybrid solar energy conversion system Photocatalytic overall seawatersplitting Thermoelectric power generation Phase change materials All-day operation

Coordination structure regulation in non-flammable electrolyte enabling high voltage lithium electrochemistry

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Journal of energy Chemistry 2024年第9期96卷 282-290页

作者： Zhiwen Deng Ye Jia Yan Deng Changhaoyue Xu Xuemei Zhang Qiujie He Jianan Peng Hao Wu Wenlong Cai College of Materials Science and Engineering Sichuan UniversityChengdu 610064SichuanChina Engineering Research center of alternative energy Materials and Devices Sichuan UniversityChengdu 610064SichuanChina

High-voltage battery systems bring significant increases in energy density but are also accompanied by fast degradation of electrochemical performance and serious safety ***,Li^(+)coordination structure regulation was conducted to formulate a non-flammable electrolyte,which consists of 1.5 M lithium bis(fluor sulfonyl)imide(LiFSI)in triethyl phosphate and methyl 2,2,2-trifluoromethyl carbonate(FEMC).The renamed TEP-FEMC-FEC(TFF)electrolyte exhibits an FSI^(−)-dominated solvation structure contributed by the weakly-solvating ability of *** generated inorganic-rich interfacial layers are conducive to stabilizing the phase transition of high-voltage cathodes while suppressing the dendritic growth on lithium metal or co-intercalation behavior in graphite *** TFF electrolyte enables LiCoO_(2)||Li batteries to achieve capacity maintenance over 79%after 400 cycles with high-rate of 5 C at an ultra-high voltage of 4.6 V,and an outstanding capacity exceeding 100 mA h g^(−1)even at a super-high current density of 20 ***,the Ah-level LiCoO_(2)||graphite pouch cells also exhibit high capacity retention and satisfactory safety performance even under fast *** work provides a novel research direction for the pursuit of high energy density non-flammable electrolytes.

关键词： Non-flammable Solvation structure High-voltage Lithium batteries

Crystalline carbon nitride with in-plane built-in electric field accelerates carrier separation for excellent photocatalytic hydrogen evolution

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Chinese Chemical Letters 2024年第4期35卷 160-165页

作者： Wengao Zeng Yuchen Dong Xiaoyuan Ye Ziying Zhang Tuo Zhang Xiangjiu Guan Liejin Guo International Research center for renewable energy State Key Laboratory of Multiphase Flow in Power EngineeringXi'an Jiaotong UniversityXi'an 710049China

Achieving a high carrier migration efficiency by constructing built-in electric field is one of the promising approaches for promoting photocatalytic activity. Herein, we have designed a donor-acceptor(D-A) crystalline carbon nitride(APMCN) with 4-amino-2,6-dihydroxypyrimidine(AP) as electron donor, in which the pyrimidine ring was well embedded in the heptazine ring via hydrogen-bonding effect during hydrothermal process. The APMCN shows superior charge-transfer due to giant built-in electric field(5.94times higher than pristine carbon nitride), thereby exhibiting excellent photocatalytic H_(2) evolution rate(1350 μmol/h) with a high AQY(62.8%) at 400 nm. Mechanistic analysis based on detailed experimental investigation together with theoretical analysis reveals that the excellent photocatalytic activity is attributed to the promoted charge separation by the giant internal electric field originated from the D–A structure.

关键词： Crystalline carbon nitride Built-in electric field Donor-acceptor structure Photocatalysis Hydrogen production

ZnO/ZnS heterostructure in N-doped porous carbon for anchoring-diffusion-conversion of polysulfides for high-performance lithium-sulfur batteries

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Rare Metals 2024年第8期43卷 3661-3676页

作者： Fei Wang Rong-Wei Huang Wen-Chang Han Chun-Man Yang Wen-Hao Yang Peng Dong Chao-Ling Wu Yi-Yong Zhang Xue Li Ying-Jie Zhang National Local Joint Engineering Research center for LithiumIon Batteries and Materials Preparation Technology Key Laboratory of Advanced Batteries Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China Engineering Research center of alternative energy Materials and Devices Sichuan UniversityMinistry of EducationChengdu 610065China

The shuttle effect of polysulfides is one of the key factors hindering the commercialization of lithiumsulfur batteries(LSBs).Owing to their high conductivity and advantageous structure,heterostructures can be used in sulfur fixation and catalysis of *** this study,a flower-shaped ZnO/ZnS heterostructure on a nitrogendoped porous carbon(NPC) sulfur host was *** ZnO/ZnS heterostructure regulates the electronic structure of the material and exhibits higher metal-like ***,the ZnO/ZnS heterostructure combines the strong adsorption property of ZnO and the high catalytic ability of ZnS to realize the anchoring-diffusionconversion of lithium poly sulfides(LiPSs).Results reveal that the developed ZnO/ZnS@NPC/S cathode has excellent electrochemical performance in LSBs,achieving a high discharge specific capacity of 1365.3 mAh·g^(-1) at 0.1C and excellent rate capability(719 mAh·g^(-1) at 2C;the capacity decay rate is only 0.042% per cycle after 1000 cycles).Even under a high sulfur loading-E/S(electrolyte/sulfur)ratio of 5.1 mg·cm^(-2)-6 μl·mg^(-1),a high specific capacity of 723.7 mAh·g^(-1) is maintained after 60 *** study provides a new strategy for a multifunctional sulfur host that can effectively alleviate the shuttle effect of LiPSs and improve the utilization of sulfur active substances.

关键词： ZnO/ZnS heterostructure Lithium-sulfur batteries Density functional theory Anchor Conversion

Recent progress in thermodynamic and kinetics modification of magnesium hydride hydrogen storage materials

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Materials Reports(energy) 2024年第1期4卷 3-22页

作者： Yafei Liu Yusang Guo Yaru Jiang Lizhuang Feng Yu Sun Yijing Wang Key Laboratory of Advanced energy Materials Chemistry Ministry of EducationRenewable Energy Conversion and Storage CenterCollege of ChemistryCollaborative Innovation Center of Chemical Science and Engineering(Tianjin)Nankai UniversityTianjin300071PR China

Hydrogen energy has emerged as a pivotal solution to address the global energy crisis and pave the way for a cleaner,low-carbon,secure,and efficient modern energy system.A key imperative in the utilization of hydrogen energy lies in the development of high-performance hydrogen storage ***-based hydrogen storage materials exhibit remarkable advantages,including high hydrogen storage density,cost-effectiveness,and abundant magnesium resources,making them highly promising for the hydrogen energy ***,practical applications of magnesium hydride for hydrogen storage face significant challenges,primarily due to their slow kinetics and stable thermodynamic ***,we briefly summarize the thermodynamic and kinetic properties of MgH2,encompassing strategies such as alloying,nanoscaling,catalyst doping,and composite system construction to enhance its hydrogen storage ***,nanoscaling and catalyst doping have emerged as more effective modification *** discussion focuses on the thermodynamic changes induced by nanoscaling and the kinetic enhancements resulting from catalyst *** emphasis lies in the synergistic improvement strategy of incorporating nanocatalysts with confinement materials,and we revisit typical works on the multi-strategy optimization of *** conclusion,we conduct an analysis of outstanding challenges and issues,followed by presenting future research and development prospects for MgH2 as hydrogen storage materials.

关键词： Magnesium hydride Thermodynamics and kinetics Catalyst doping Nanostructures Hydrogenation and dehydrogenation