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Green Chemical Engineering 2022年第1期3卷 64-70页

作者： Jianguo Liu Yanpei Song Huanli Wang Longlong Ma key laboratory of energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing210096China Dalian National laboratory for Clean energy Dalian116023China CAS key laboratory of renewable energy Guangdong Provincial Key Laboratory of New and Renewable Energy Research and DevelopmentGuangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou510640China

Development of the economic, environmentally friendly synthesis of amines from nitro compounds remains important and challenging. In this work, the graphene shell encapsulated none noble Ni-based catalysts were successfully designed and synthesized via an environmentally friendly method using H2O or Et OH as solvent. These fresh and recycling catalysts were characterized by X-ray diffraction and X-ray photoelectron spectroscopy. For the nitro compounds hydrogenation, Ni@C-600-H2O exhibits the best catalytic activity to achieve 100 mol/mol conversions of nitrobenzene and 99% selectivity of aniline under mild reaction conditions of 1.0 MPa H2and 60°C.Many halogen-substituted, olefin substituted nitro compounds and aliphatic nitro compounds were investigated and desired products were obtained in excellent selectivity. What is more, the catalyst had excellent stability and could be recycled 13 times without any significant loss in selectivity and activity. Furthermore, we also reported the methodology for tertiary amines synthesis using Ni-based catalyst via one-pot, cost-effective tandem combination reaction with nitrobenzene hydrogenation and amines N-methylation.

关键词： Encapsulated graphene shell Ni@graphene catalyst Selective hydrogenation Nitro compounds

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,etc.Major 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 co-catalysts.Therefore,it is desirable yet challenging to explore a highly selective and efficient oxydehydrogenation capacity for DHIQ synthesis under eco-friendly reaction conditions.Herein,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%,respectively.Cu 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 conditions.The corresponding catalytic activity can maintain at least five recyclings and can be further applied to gram-scale experiments.Additionally,the efficient preparation of DHIQ catalyzed by Cu NPs@1-3 could be realized even under air conditions.Importantly,the anticancer molecule precursor synthesis of 6,7-dimethoxy-3,4-dihydroisoquinoline was also selectively catalyzed by Cu NPs@1-3.Mechanism 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 centers.More 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

A novel flow-resistor network model for characterizing enhanced geothermal system heat reservoir

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Frontiers in energy 2019年第1期13卷 99-106页

作者： Jian GUO Wenjiong CAO Yiwei WANG Fangming JIANG laboratory of Advanced energy Systems of CAS key laboratory of renewable energy and Guangdong Key Laboratory of New and Renewable Energy Research and DevelopmentGuangzhou Institute of Energy Conversion.Chinese Academy of Sciences(CAS)Guangzhou 510640China

The fracture characteristics of a heat reservoir are of critical importance to enhanced geothennal systems,which can be investigated by theoretical modeling.This paper presents the development of a novel flow.Fesistor network model to describe the hydraulic processes in heat reservoirs.The fractures in the reservoir are simplified by using flow resistors and the typically complicated fracture network of the heat reservoir is converted into a flowresistor network with a reasonably simple pattern.For heat reservoirs with various fracture configurations,the corresponding flow-resistor networks are identical in terms of framework though the networks may have difftrent section numbers and the flow resistors may have different values.In this paper,numerous cases of different section numbers and resistor values are calculated and the results indicate that the total number of flow resistances between the injection and production wells is primarily determined by the number of fractures in the reservoir.It is also observed that a linear dependence of the total flow resistance on the number of fractures and the relation is obtained by the best fit of the calculation results.Besides,it perfbmis a case study dealing with the Soultz enhanced geothermal system(EGS).In addition,the fracture numbers underneath specific well systems are derived.The results provide in sight on the tortuosity of the flow path betwee n different wells.

关键词： enhanced geothennal systems flow-resistor network model fracture characteristics heat reservoir

Protonated and layered transition metal oxides as solid acids for dehydration of biomass-based fructose into 5-hydroxymethylfurfural

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Journal of energy Chemistry 2017年第1期26卷 147-154页

作者： Jiawei Zhong Yuanyuan Guo Jinzhu Chen key laboratory of renewable energy Guangdong Key Laboratory of New and Renewable Energy Research and Development Guangzhou Institute of Energy Conversion Chinese Academy of Sciences University of Chinese Academy of Sciences

A serial of protonated and layered transition metal oxides, including layered HTaWO6, HNbMoO6 as well as HNbWO6, were synthesized by solid-state reaction and ion-exchange. The layered HTaWO6 has been systematically studied as a solid acid to realize the dehydration of fructose to 5-hydroxymethylfurfural (HMF). The transition metal oxide samples were characterized with ICP-OES, EDS, XRD, XPS, SEM, TGA, FT-IR, N-2 adsorption-desorption and NH3-TPD. The influential factors such as reaction temperature, reaction time, solvent, catalyst amount and substrate concentration were deeply investigated. The optimized fructose conversion rate of 99% with HMF yield of 67% were achieved after 30 min at 140 degrees C in dimethylsulfoxide. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.

关键词： Biomass Dehydration 5-HYdroxymethylfurfural Layered transition metal oxide Solid acid

Facile synthesis of hydrochar-supported catalysts from glucose and its catalytic activity towards the production of functional amines

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Green energy & Environment 2023年第5期8卷 1358-1370页

作者： Xiuzheng Zhuang Jianguo Liu Longlong Ma key laboratory of energy Thermal Conversion and Control of Ministry of Education School of Energy and EnvironmentSoutheast UniversityNanjing210096China key laboratory of renewable energy Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou510640China

Since the utilization of abundant biomass to develop advanced materials has become an utmost priority in recent years,we developed two sustainable routes(i.e.,the impregnation method and the one-pot synthesis)to prepare the hydrochar-supported catalysts and tested its catalytic performance on the reductive amination.Several techniques,such as TEM,XRD and XPS,were adopted to characterize the structural and catalytic features of samples.Results indicated that the impregnation method favors the formation of outer-sphere surface complexes with porous structure as well as well-distributed metallic nanoparticles,while the one-pot synthesis tends to form the inner-sphere surface complexes with relatively smooth appearance and amorphous metals.This difference explains the better activity of catalysts prepared by the impregnation method which can selectively convert benzaldehyde to benzylamine with an excellent yield of 93.7%under the optimal reaction conditions;in contrast,the catalyst prepared by the one-pot synthesis only exhibits a low selectivity near to zero.Furthermore,the gram-scale test catalyzed by the same catalysts exhibits a similar yield of benzylamine in comparison to its smaller scale,which is comparable to the previously reported heterogeneous noble-based catalysts.More surprisingly,the prepared catalysts can be expediently recycled by a magnetic bar and remain the satisfying catalytic activity after reusing up to five times.In conclusion,these developed catalysts enable the synthesis of functional amines with excellent selectivity and carbon balance,proving cost-effective and sustainable access to the wide application of reductive amination.

关键词： Impregnation method One-pot synthesis Hydrochar-supported catalyst Reductive amination

A Lightweight Compact Lithium-Ion Battery Thermal Management System Integratable Directly with EV Air Conditioning Systems

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Journal of Thermal Science 2022年第6期31卷 2363-2373页

作者： LIN Bichao CEN Jiwen JIANG Fangming laboratory of Advanced energy Systems Guangzhou Institute of Energy ConversionChinese Academy of SciencesGuangzhou510640China CAS key laboratory of renewable energy Guangzhou 510640China Guangdong Provincial key laboratory of New and renewable energy Research and Development Guangzhou 510640China University of Chinese Academy of Sciences Beijing 100049China

This paper discusses an improved thermal management system to ameliorate the performance of lithium-ion battery storage systems for electric vehicles(EVs) applications. A compact and lightweight cold plate is designed and fabricated to fit 18650-type lithium-ion batteries, using aluminum-finned copper tubes. A dynamic temperature PID(proportional, integral, differential) control algorithm for electronic expansion valves is developed to study using EV air conditioning refrigerant, R134a, to control battery modules’ temperature with this compact and lightweight thermal management system. The experimental results show that the proposed battery thermal management system can effectively control the battery module’s temperature. In addition, during 1C discharge, when the PID temperature algorithm control scheme is used, the maximum temperature difference across the battery module peaks at less than 4℃, and the maximum temperature within the battery module is less than 36℃.

关键词： electric vehicles air conditioning system battery thermal management finned tube two-phase flow

Cobalt coordination modified double-schiff-base with low solubility as a long-cycle life anode for sodium-ion batteries

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Progress in Natural Science:Materials International 2022年第4期32卷 510-516页

作者： Mengyuan Yue Huinan Guo Zhaoxia Yuan Weiqin Li Yafei Liu Kai Chen Yusang Guo Yijing Wang key laboratory of Advanced energy Materials Chemistry (Ministry of Education) Renewable Energy Conversion and Storage Center College of Chemistry Nankai University

Sodium-ion batteries(SIBs) have been recently considered as an intriguing candidate for next-generation battery systems with their advantages in large-scale energy storage applications. However, the design of electrode materials of SIBs still suffers from severe volume expansion and low capacity caused by the larger ion radius, high redox potential and heavy atom weight of Na. Organic electrode materials with structural flexibility have attracted great attention recently for their potential in alleviating volume expansion. However, most organic electrode materials suffer from dissolution in electrolytes and consequent capacity fading during the long-term cycling process. In this work, a method coordinating with Co2+was applied to solve the shuttle effect of H4salphdc(N, N’-phenylene-bis-(salicylideneimine) dicarboxylic acid). By virtue of the Co2+coordination, the Co(H2salphdc)electrode delivered a desirable discharge capacity of 123 m Ah g-1after 1500 cycles at the current density of 200m A g-1, while the H4salphdc electrode exhibited severe capacity fading. Such excellent electrochemical performance can be credited to the Co2+coordination repressing the electrode dissolution and improving the structure stability.

关键词： Double-Schiff-base Sodium-ion battery Shuttle effects

Dependence of Size and Morphology on Shear Flow for PS-based Amphiphilic Block Copolymer Micelles in Aqueous Solution

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Chinese Journal of Polymer Science 2017年第5期35卷 641-648页

作者：王志达 Chang-feng Yan Ying Huang Li-qi Yi key laboratory of renewable energy Guangzhou Institute of Energy ConversionChinese Academy of Sciences Guangdong key laboratory of New and renewable energy Research and Development University of Chinese Academy of Sciences

This contribution focuses on the impact of shear flow on size and nanostructure of PS-based amphiphilic block copolymer （BC） micelles by varying the stirring rate and copolymer composition. The results show that the vesicles formed from diblock copolymer （di-BC） of PS-b-PAA remain with vesicular morphology, although the average size decreases, with the increase of stirring rate. However, the multi-compartment micelles （MCMs） formed from tri-block copolymer （tri-BC） of PS-b-P2VP-b-PEO are quite intricate, in which the copolymer first self-assembles into spheres, then to clusters, to large compound micelles （LCMs）, and finally back to spheres, as stirring rate increases from 100 r/min to 2200 r/min. Formation mechanism studies manifest that vesicles form simultaneously as water is added to the di-BC solution, termed as direct- assembly, and remain with vesicular structure in the flowing process. While for the PS-b-P2VP-b-PEO copolymer, spherical micelles at initial stage can further assemble into clusters and LCMs, termed as second-assembly, due to the speeding-up- aggregation of the favorable stirring. As a result, an invert V-relationship between tri-BC micelle dimension and stirring rate is observed in contrast to the non-linear decreasing curve of di-BC vesicles. It is by investigating these various amphiphilic BCs that the understanding of shear dependence of size and morphology of micelles is improved from self-assembly to second-assembly process.

关键词： Self-assembly Shear Size Nanostructure Block copolymer

N,N-dimethylformamide tailors solvent effect to boost Zn anode reversibility in aqueous electrolyte

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National Science Review 2022年第10期9卷 147-157页

作者： Yilin Ma Qiu Zhang Luojia Liu Yixin Li Haixia Li Zhenhua Yan Jun Chen key laboratory of Advanced energy Materials Chemistry (Ministry of Education) Renewable Energy Conversion and Storage Center (RECAST) College of Chemistry Nankai University

Rechargeable aqueous Zn batteries are considered as promising energy-storage devices because of their high capacity,environmental friendliness and low cost.However,the hydrogen evolution reaction and growth of dendritic Zn in common aqueous electrolytes severely restrict the application of Zn batteries.Here,we develop a simple strategy to suppress side reactions and boost the reversibility of the Zn electrode.By introducing 30%(volume fractions) N,N-dimethylformamide(DMF) to the 2 M Zn(CF3SO3)2-H2O electrolyte(ZHD30),the preferential hydrogen-bonding effect between DMF and H2O effectively reduces the water activity and hinders deprotonation of the electrolyte.The ZHD30 electrolyte improves the Zn plating/stripping coulombic efficiency from～95.3% to～99.4% and enhances the cycles from 65 to 300.The Zn-polyaniline full battery employing the ZHD30 ele ctrolyte can operate over a wide temperature range from-40℃ to+25℃ and deliver capacities of 161.6,127.4 and 65.8 mAh g-1at 25,-20 and-40℃,respectively.This work provides insights into the role of tuning solvent effects in designing low-cost and effective aqueous electrolytes.

关键词： aqueous electrolyte Zn reversibility hydrogen bond solvent effect rechargeable Zn battery

Effect of catalyst layer mesoscopic pore-morphology on cold start process of PEM fuel cells

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Frontiers in energy 2021年第2期15卷 460-472页

作者： Ahmed Mohmed DAFALLA Fangming JIANG laboratory of Advanced energy Systems Guangdong Key Laboratory of New and Renewable Energy Research and DevelopmentCAS Key Laboratory of Renewable EnergyGuangzhou Institute of Energy ConversionChinese Academy of Sciences(CAS)Guangzhou 510640China University of Chinese Academy of Sciences Beijing 100049China

Water transport is of paramount importance to the cold start of proton exchange membrane fuel cells(PEMFCs).Analysis of water transport in cathode catalyst layer(CCL)during cold start reveals the distinct characteristics from the normal temperature operation.This work studies the effect of CCL mesoscopic pore-morphology on PEMFC cold start.The CCL mesoscale morphology is characterized by two tortuosity factors of the ionomer network and pore structure,respectively.The simulation results demonstrate that the mesoscale morphology of CCL has a significant influence on the performance of PEMFC cold start.It was found that cold-starting of a cell with a CCL of less tortuous mesoscale morphology can succeed,whereas starting up a cell with a CCL of more tortuous mesoscale morphology may fail.The CCL of less tortuous pore structure reduces the water back diffusion resistance from the CCL to proton exchange membrane(PEM),thus enhancing the water storage in PEM,while reducing the tortuosity in ionomer network of CCL is found to enhance the water transport in and the water removal from CCL.For the sake of better cold start performance,novel preparation methods,which can create catalyst layers of larger size primary pores and less tortuous pore structure and ionomer network,are desirable.

关键词： cold start energy conversion fuel cells mesoscale morphology tortuosity water management