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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

Rotor Angle Stability Prediction Using Temporal and Topological Embedding Deep Neural Network Based on Grid-informed Adjacency Matrix

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Journal of Modern Power Systems and Clean energy 2024年第3期12卷 695-706页

作者： Peiyuan Sun Long Huo Xin Chen Siyuan Liang the School of Electrical Engineering Xi’an Jiaotong UniversityXi’an 710049China the School of Electrical Engineering and the Center of Nanomaterials for Renewable EnergyState Key Laboratory of Electrical Insulation and Power EquipmentXi’an Jiaotong UniversityXi’an 710049China the Department of Computer Science and Engineering The Chinese University of Hong KongShatin999077Hong KongChina

Rotor angle stability(RAS)prediction is critically essential for maintaining normal operation of the interconnected synchronous machines in power *** wide deployment of phasor measurement units(PMUs)promotes the development of data-driven methods for RAS *** paper proposes a temporal and topological embedding deep neural network(TTEDNN)model to accurately and efficiently predict RAS by extracting the temporal and topological features from the PMU *** grid-informed adjacency matrix incorporates the structural and electrical parameter information of the power *** the small-signal RAS with disturbance under initial operating conditions and the transient RAS with short circuits on transmission lines are *** studies of the IEEE 39-bus and IEEE 300-bus power systems are used to test the performance,scalability,and robustness against measurement uncertainties of the TTEDNN *** show that the TTEDNN model performs best among existing deep learning ***,the superior transfer learning ability from small-signal RAS conditions to transient RAS conditions has been proved.

关键词： Rotor angle stability prediction topological embedding deep learning graph convolution network

Copper-induced formation of heterostructured Co_(3)O_(4)/CuO hollow nanospheres towards greatly enhanced lithium storage performance

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Chinese Chemical Letters 2024年第2期35卷 594-598页

作者： Junjun Zhang Huiying Lu Tianhao Yao Xin Ji Qingmiao Zhang Lingjie Meng Jianmin Feng Hongkang Wang College of Geography & Environment Xianyang Normal UniversityXianyang 712000China State Key Lab of Electrical Insulation and Power Equipment Center of Nanomaterials for Renewable Energy (CNRE)School of Electrical EngineeringXi'an Jiaotong UniversityXi'an 710049China School of Chemistry Xi'an Key Laboratory of Sustainable Energy Material Chemistryand Instrumental Analysis CenterXi'an Jiaotong UniversityXi'an 710049China

We report a facile template-free fabrication of heterostructured Co_(3)O_(4)/CuO hollow nanospheres using pre-synthesized Co/Cu-glycerate as conformal *** introduction of copper nitrate in the solvothermal reaction system of glycerol/isopropanol/cobalt nitrate readily induces the conversion from solid Co-glycerate to hollow Co/Cu-glycerate nanospheres,and the effect of the Co/Cu atomic ratio on the structure evolution of the metal glycerates as well as their corresponding oxides were *** examined as anode materials for lithium-ion batteries,the well-defined Co_(3)O_(4)/CuO hollow nanospheres with Co/Cu molar ratio of 2.0 demonstrate excellent lithium storage performance,delivering a high reversible capacity of 930 mAh/g after 300 cycles at a current density of 0.5 A/g and a stable capacity of 650 mAh/g after 500 cycles even at a higher current density of 2.0 A/g,which are much better than their counterparts of bare CuO and Co_(3)O_(4).The enhanced lithium storage performance can be attributed to the synergistic effect of the CuO and Co_(3)O_(4)heterostructure with hollow spherical morphology,which greatly enhances the charge/electrolyte transfer and effectively buffers the volume changes upon lithiation/delithiation cycling.

关键词： Lithium-ion batteries Co/Cu-glycerate Hollow nanospheres Co_(3)O_(4)/CuO heterostructure Electrochemical properties

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

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

Heterostructure Cu_(3)P-Ni_(2)P/CP catalyst assembled membrane electrode for high-efficiency electrocatalytic nitrate to ammonia

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Nano Research 2024年第6期17卷 4872-4881页

作者： Meng Jin Jiafang Liu Xian Zhang Shengbo Zhang Wenyi Li Dianding Sun Yunxia Zhang Guozhong Wang Haimin Zhang Laboratory of Materials Physics Centre for Environmental and Energy NanomaterialsAnhui Key Laboratory of Nanomaterials and NanotechnologyCAS Center for Excellence in NanoscienceInstitute of Solid State PhysicsHefei Institutes of Physical ScienceChinese Academy of SciencesHefei 230031China University of Science and Technology of China Hefei 230026China Anhui Contango New energy Technology Co. Ltd.Hefei 230031China

Electrochemical nitrate reduction reaction(NO_(3)RR)is a promising means for generating the energy carrier ***,we report the synthesis of heterostructure copper-nickel phosphide electrocatalysts via a simple vapor-phase hydrothermal *** resultant catalysts were evaluated for electrocatalytic nitrate reduction to ammonia(NH_(3))in three-type electrochemical *** detail,the regulation mechanism of the heterogeneous Cu_(3)P-Ni_(2)P/CP-x for NO_(3)RR performance was systematically studied through the H-type cell,rotating disk electrode setup,and membrane-electrode-assemblies(MEA)*** a result,the Cu_(3)P-Ni_(2)P/CP-0.5 displays the practicability in an MEA system with an anion exchange membrane,affording the largest ammonia yield rate(RNH_(3))of 1.9 mmol·h^(−1)·cm^(−2),exceeding most of the electrocatalytic nitrate reduction electrocatalysts reported to *** theoretical calculations and in-situ spectroscopy characterizations uncover that the formed heterointerface in Cu_(3)P-Ni_(2)P/CP is beneficial for promoting nitrate adsorption,activation,and conversion to ammonia through the successive hydrodeoxygenation pathway.

关键词： electrocatalytic nitrate reduction to ammonia three-type reactors membrane-electrode-assemblies system operando ATR-IRRAS successive hydrodeoxygenation pathway