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Room-temperature fast assembly of 3D macroscopically porous graphene frameworks for binder-free compact supercapacitors with high gravimetric and volumetric capacitances

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Journal of Energy Chemistry 2021年第10期30卷 23-28,I0002页

作者： Sen Wang Xiao Wang chenglin sun Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023LiaoningChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of Sciences457 Zhongshan RoadDalian 116023LiaoningChina University of Chinese Academy of Sciences Shijingshan District19 A Yuquan RdBeijing 100049China

Synthesis and applications of three-dimensional(3 D)porous graphene frameworks(GFs)have attracted extensive interest owing to their intriguing advantages of high specific surface area,enriched porosity,excellent electrical conductivity,exceptional compressibility and ***,it is still challenging for economically viable,fast and scalable assembly of 3 D GFs at ***,we reported a one-step scalable strategy for fast self-assembly of graphene oxide into 3 D macroscopically porous GFs,with assistance of polyoxometalates(POM)as functional cross-linker and hydrazine hydrate as reductant at *** resulting 3 D interconnected macroporous POM-GFs uniformly decorated with ultrasmall POM nanoclusters were directly processed into binder-/additive-free film compact electrodes(1.68 g cm^(-3))with highly aligned,layer-stacked structure and electrically conductivity(622 S m-1)for high-performance supercapacitors,showing an impressive gravimetric capacitance of205 F g-1,volumetric capacitance of 334 F cm^(-3) at 1 mV s^(-1),and remarkable cycling stability with capacitance retention of 83%after 10,000 cycles,outperforming the most reported ***,the solid-state supercapacitors offered excellent gravimetric capacitance of 157 F g-1 exceptionally volumetric capacitance of 115 F cm^(-3) at 2 mV s^(-1) based on single electrode,and volumetric energy density of2.6 mWh cm^(-3).Therefore,this work will open novel opportunities to room-temperature fast assembly of 3 D porous graphene architectures for high-energy-density supercapacitors.

关键词： Graphene frameworks Room-temperature fast assembly Supercapacitors

Recent progress of dendrite-free stable zinc anodes for advanced zinc-based rechargeable batteries:Fundamentals,challenges,and perspectives

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SusMat 2023年第2期3卷 180-206页

作者： Xiao Wang chenglin sun Zhong-Shuai Wu State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalianChina

Zinc-based batteries are a very promising class of next-generation electrochemical energy storage systems,with high safety,eco-friendliness,abundant resources,and the absence of rigorous manufacturing ***,practical applications of zinc-based rechargeable batteries are impeded by the low Coulombic efficiency,inferior cyclability,and poor rate capability,due to the instability of zinc ***,effective strategies for dendritefree zinc anode are symmetrically reviewed,especially highlighting specific mechanisms,delicate design of electrode and current collectors,controlled electrode|electrolyte interface,ameliorative electrolytes,and advanced separators ***,the particular mechanisms of dendrites formation and the associated fundamentals of the stable Zn metal anodes are presented ***,recent key strategies for dendrites prevention and hydrogen evolution reaction suppression are categorized,discussed,and analyzed in detail in view of the electrodes,electrolytes,and ***,the challenging perspectives and major directions of stable zinc anodes are briefly discussed for further industrialization and commercialization of zinc-based rechargeable batteries.

关键词： dendrite-free mechanisms zinc anode zinc ion batteries

Use of catalytic wet air oxidation (CWAO) for pretreatment of high-salinity high-organic wastewater

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Journal of Environmental Sciences 2022年第10期34卷 105-114页

作者： Wenjing sun Hongxia Lv Lei Ma Xiangdong Tan Chengyu Jin Huiling Wu Lili Chen Mengyang Liu Huangzhao Wei chenglin sun Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology College of Chemical EngineeringBeijing Institute of Petrochemical TechnologyBeijing 102617China University of Chinese Academy of Sciences Beijing 100049China

Catalytic wet air oxidation(CWAO)coupled desalination technology provides a possibility for the effective and economic degradation of high salinity and high organic *** widely occurs in natural and wastewaters,and its high content jeopardizes the efficacy of Advanced oxidation process(AOPs).Thus,a novel chlorine ion resistant catalyst Bsite Ru doped LaFe_(1-x)Ru_(x)O_(3-)δin CWAO treatment of chlorine ion wastewater was ***,LaFe_(0.85)Ru_(0.15)O_(3-δ)was 45.5% better than that of the 6%RuO_(2)@TiO_(2)(commercial carrier)on total organic carbon(TOC)***,doped catalysts LaFe_(1-x)Ru_(x)O_(3-)δshowed better activity than supported catalysts RuO_(2)@LaFeO_(3) and RuO_(2)@TiO_(2) with the same Ru ***,LaFe_(0.85)Ru_(0.15)O_(3-)δhas novel chlorine ion resistance no matter the concentration of Cl^(−) and no Ru dissolves after the reaction.X-ray diffraction(XRD)refinement,X-ray photoelectron spectroscopy(XPS),transmission electron microscope(TEM),and X-ray absorption fine structure(XAFS)measurements verified the structure of LaFe_(0.85)Ru_(0.15)O_(3-)δ.Kinetic data and density functional theory(DFT)proved that Fe is the site of acetic acid oxidation and adsorption of chloride *** existence of Fe in LaFe_(0.85)Ru_(0.15)O_(3-)δcould adsorb chlorine ion(catalytic activity inhibitor),which can protect the Ru site and other active oxygen species to exert catalytic *** work is essential for the development of chloride-resistant catalyst in CWAO.

关键词： Catalytic wet air oxidation Heterogeneous catalysis LaFe_(1-x)Ru_(x)O_(3-)δ Chlorine wastewater Salt resistance mechanism

The high catalytic activity and strong stability of 3%Fe/AC catalysts for catalytic wet peroxide oxidation of m-cresol: The role of surface functional groups and FeO_(x) particles

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Chinese Journal of Chemical Engineering 2022年第4期35卷 105-114页

作者： Peiwei Han Chunhua Xu Yamin Wang chenglin sun Huangzhao Wei Haibo Jin Ying Zhao Lei Ma Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology/College of Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China Shandong Key Laboratory of Water Pollution Control and Resource Reuse School of Environmental Science and EngineeringShandong UniversityQingdao 266237China Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China

FeO;supported on activated carbon(AC) has been shown to be an ideal catalyst for catalytic wet peroxide oxidation(CWPO) due to its high CWPO reaction activity and stability. Although there have been some studies on the mechanism of Fe/AC catalysis in CWPO, the specific contribution of each component(surface oxygen groups and FeOxon AC) inside an Fe/AC catalyst and their corresponding reaction mechanism remain unclear, and the reaction stability of CWPO catalysts has rarely been discussed. Then the optimal CWPO catalyst in our laboratory, 3%Fe/AC, was selected.(1) By removing certain components on the AC through heat treatment, its contribution to the reaction and the corresponding reaction mechanism were investigated. With the aid of temperature-programmed desorption–mass spectrometry(TPD–MS) and the CWPO reaction, the normalized catalytic contributions of components were shown to be: 37.3%(carboxylic groups), 5.3%(anhydride), 19.3%(ether/hydroxyl),-71.4%(carbonyl groups) and 100%(FeOx),respectively. DFT calculation and EPR analysis confirmed that carboxylic groups and Fe_(2)O_(3) are able to activate the H_(2)O_(2) to generate·OH.(2) The catalysts at were characterized at different reaction times(0 h, 450 h, 900 h, 1350 h, and 1800 h) by TPD–MS and M?ssbauer spectroscopy. Results suggested that the number of carboxylic goups gradually increased and the size of paramagnetic Fe_(2)O_(3) particle crystallites gradually increased as the reactions progressed. The occurrence of strong interactions between metal oxides and AC was also confirmed. Due to these effects, the strong stability of 3%Fe/AC was further improved. Therefore, the reasons for the high activity and strong stability of 3%Fe/AC in CWPO were clearly shown. We believe that this work provides an idea of the removal of cresols from wastewater into the introduction to show the potential applications of CWPO.

关键词： Catalytic wet peroxide oxidation Fe/AC catalyst Surface functional groups Reaction mechanism

Life cycle assessment of high concentration organic wastewater treatment by catalytic wet air oxidation

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Chinese Journal of Chemical Engineering 2023年第4期56卷 80-88页

作者： Yuxi Chai Yanan Zhang Yannan Tan Zhiwei Li Huangzhao Wei chenglin sun Haibo Jin Zhao Mu Lei Ma Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology/College of New Materials and Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China School of Chemistry and Chemical Engineering Hefei University of TechnologyHefei 230009China Institute of Applied Chemical Technology for Oilfield/College of New Materials and Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China

There have been many studies on life cycle assessment in sewage treatment,but there are scarce few studies on the treatment of industrial wastewater in combination with advanced oxidation technology,especially in catalytic wet air oxidation(CWAO).There are no cases of using actual industrialized data onto life cycle *** paper uses Simapro 9.0 software to establish a life cycle assessment model for the treatment of high-concentration organic wastewater by CWAO,and comprehensively explains the impact on the environment from three aspects:the construction phase,the operation phase and the demolition *** addition,sensitivity analysis and uncertainty analysis were *** results showed that the key factors affecting the environment were marine ecotoxicity,mineral resource consumption and global warming,the operation stage had the greatest impact on the environment,which was related to high power consumption during operation and emissions from the treatment *** analysis showed that electricity consumption has the greatest impact on abiotic depletion and freshwater aquatic ecotoxicity,and it also proved that global warming is mainly caused by pollutant emissions during operation *** Carlo simulations found slightly higher uncertainty for abiotic depletion and toxicity-related impact categories.

关键词： Wastewater treatment High-concentration organic wastewater Catalytic wet air oxidation Life-cycle assessment

Scalable fabrication of printed Zn//MnO2 planar micro-batteries with high volumetric energy density and exceptional safety

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National Science Review 2020年第1期7卷 64-72页

作者： Xiao Wang Shuanghao Zheng Feng Zhou Jieqiong Qin Xiaoyu Shi Sen Wang chenglin sun Xinhe Bao Zhong-Shuai Wu Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences University of Chinese Academy of Sciences State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Department of Chemical Physics University of Science and Technology of China

The rapid development of printed and microscale electronics imminently requires compatible micro-batteries（MBs） with high performance, applicable scalability, and exceptional safety, but faces great challenges from the ever-reported stacked geometry. Herein the first printed planar prototype of aqueous-based, high-safety Zn//MnO2MBs, with outstanding performance, aesthetic diversity, flexibility and modularization, is demonstrated, based on interdigital patterns of Zn ink as anode and MnO2ink as cathode, with high-conducting graphene ink as a metal-free current collector, fabricated by an industrially scalable screen-printing technique. The planar separator-free Zn//MnO2MBs, tested in neutral aqueous electrolyte, deliver a high volumetric capacity of 19.3 mAh/cm3（corresponding to 393 mAh/g） at 7.5 mA/cm3, and notable volumetric energy density of 17.3 mWh/cm3, outperforming lithium thin-film batteries（≤10 mWh/cm3）. Furthermore, our Zn//MnO2MBs present long-term cyclability having a high capacity retention of 83.9% after 1300 cycles at 5 C, which is superior to stacked Zn//MnO2batteries previously reported. Also, Zn//MnO2planar MBs exhibit exceptional flexibility without observable capacity decay under serious deformation, and remarkably serial and parallel integration of constructing bipolar cells with high voltage and capacity output. Therefore, low-cost, environmentally benign Zn//MnO2MBs with in-plane geometry possess huge potential as high-energy, safe, scalable and flexible microscale power sources for direction integration with printed electronics.

关键词： low cost printed planar Zn//MnO2 micro-batteries metal-free current collectors

Fe_(3)C@C/C for catalytic ozonation of silicon-containing wastewater:Dual improvement of silicon resistance and catalytic effect

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Journal of Materials Science & Technology 2023年第5期136卷 65-77页

作者： Shengzhe Wang Lei Ma Rui Wang Chengyu Jin Ying Zhao Xuefei Tan Yanan Zhang Mengyang Liu Chenxing Yao Huangzhao Wei chenglin sun Dalian Institute of Chemical Physics Chinese Academy of SciencesDalian 116023China University of Chinese Academy of Sciences Beijing 100049China Beijing Key Laboratory of Fuels Cleaning and Advanced Catalytic Emission Reduction Technology/College of Chemical Engineering Beijing Institute of Petrochemical TechnologyBeijing 102617China College of Materials and Chemical Engineering Heilongjiang Institute of TechnologyHarbin 150050China School of Light Industry and Chemical Engineering Dalian Polytechnic UniversityDalian 116034China

The improvement of catalysts’stability under harsh reaction conditions is vital for their practical ***,iron carbide(Fe_(3)C)nanoparticles were encapsulated in graphitic carbon in situ and a carbon ball served as the *** synthesized Fe_(3)C@C/C was first utilized to treat an m-cresol wastewater containing Si via catalytic *** with the commercial Fe/Al_(2)O_(3)catalyst,the resistance to Si of the Fe_(3)C@C/C was improved 22.68 times,while the TOC removal rate increased by a factor of 2.9,and it remained stable during 10 cycles and 12000 min of continuous reaction,which further demon-strated its potential for diverse *** catalyst exhibits improved resistance to Si because of the dual protection from the carbon-encapsulated structure and carbon *** functional theory calculations show that the encapsulation of Fe_(3)C using carbon significantly increases the resistance to adsorption of Si on its active *** addition,the activation of O_(3)is unimpeded on the Fe_(3)C adsorption sites by the protection from C,thus the generation of reactive oxygen species(ROS)by ozone is largely *** mechanism associated with the resistance of the Fe_(3)C@C/C catalyst to Si and its elevated activity are also elucidated.

关键词： Catalytic ozonation Silicon-resistant catalyst Carbon-encapsulated Fe_(3)C@C/C Density functional theory

Scalable and fast fabrication of graphene integrated micro-supercapacitors with remarkable volumetric capacitance and flexibility through continuous centrifugal coating

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Journal of Energy Chemistry 2021年第1期30卷 284-290,I0009页

作者： Xiaoyu Shi Lijun Tian Sen Wang Pengchao Wen Ming Su Han Xiao Pratteek Das Feng Zhou Zhaoping Liu chenglin sun Zhong-Shuai Wu Xinhe Bao Department of Chemical Physics University of Science and Technology of ChinaHefei 230026AnhuiChina Great Scientific Research Institute Datong Coal Mine Group Co.LtdDatong 037003ShanxiChina Dalian National Laboratory for Clean Energy Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina State Key Laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian 116023LiaoningChina University of Chinese Academy of Sciences Beijing 100049China Ningbo Graphene Innovation Center Co. LtdNingbo 315200ZhejiangChina Ningbo Institute of Materials Technology and Engineering Chinese Academy of SciencesNingbo 315201ZhejiangChina

Microscale electrochemical energy storage devices,e.g., micro-supercapacitors(MSCs),possessing tailored performance and diversified form factors of lightweight,miniaturization,flexibility and exceptional integration are highly necessary for the smart power sources-unitized *** the great progress,the fabrication of MSCs combining high integration with high volumetric performance remains largely ***,we develop a simple,fast and scalable strategy to fabricate graphene based highly integrated MSCs by a new effective continuous centrifugal coating ***,the resulting highly conductive graphene films can act as not only patterned microelectrodes but also metal-free current collectors and interconnects,endowing modular MSCs with high integrity,remarkable flexibility,tailored voltage and capacitance output,and outstanding performance *** importantly,the strong centrifugal force and shear force generated in continuous centrifugal coating process lead to graphene films with high alignment,compactness and packing density,contributing to excellent volumetric capacitance of ~31.8 F cm^(-3) and volumetric energy density of ~2.8 mWh cm^(-3),exceeding most reported integrated ***,our work paves a novel way for simple and scalable fabrication of integrated MSCs and offers promising opportunities as standalone microscale power sources for new-generation electronics.

关键词： Integrated micro-supercapacitors Continuous centrifugal coating Graphene Flexibility Volumetric capacitance

Simplified fabrication of high areal capacitance all-solid-state micro-supercapacitors based on graphene and MnO_2 nanosheets

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Chinese Chemical Letters 2018年第4期29卷 582-586页

作者： Jieqiong Qin Zhong-Shuai Wu Feng Zhou Yanfeng Dong Han Xiao Shuanghao Zheng Sen Wang Xiaoyu Shi Haibo Huang chenglin sun Xinhe Bao Dalian National Laboratory for Clean Energy Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China State Key Laboratory of Catalysis Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 China University of Chinese Academy of Sciences Beijing 100049 China Department of Chemical Physics University of Science and Technology of China Hefei 230026 China

All-solid-state micro-supercapacitors are acknowledged as a very promising class of microscale energy storage devices for directly integrating portable and wearable electronics. However, the improvement of electrochemical performance from materials to devices still remains tremendous challenges. Here, we demonstrate a novel and universal mask-assisted filtration technology for the simplified fabrication of all-solid-state planar micro-supercapacitors（MSCs） based on interdigital patterns of 2D pseudocapacitive MnO2 nanosheets and electrochemically exfoliated graphene film as both electrode and current collector, and polyvinyl alcohol/Li Cl gel as electrolyte. Remarkably, the resulting MSCs exhibit outstanding areal capacitance of ～355 m F/cm^2, which is among the highest values reported in the state-of-the-art MSCs. Meanwhile, MSCs possess exceptionally mechanical flexibility as high as ～92% of initial capacitance even at a highly bending angle of 180°, excellent cyclability with a capacitance retention of 95% after 3000 cycles, and impressive serial or parallel integration for modulating the voltage or capacitance. Therefore, our proposed strategy of simplified construction of MSCs will pave the ways for utilizing graphene and analogous pseudocapactive nanosheets in high-performance MSCs.

关键词： MnO2 nanosheets Graphene All-solid-state Planar Micro-supercapacitors Energy storage