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PdCu alloy anchored defective titania for photocatalytic conversion of carbon dioxide into methane with 100% selectivity

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Journal of Energy Chemistry 2024年第4期91卷 254-265页

作者： lina Zhang Sajjad Hussain qiuye li Jianjun Yang National&Local Joint Engineering Research Center for Applied Technology of Hybrid Nanomaterials Henan UniversityKaifeng 475004HenanChina

The photoreduction of CO_(2)into CH_(4)with simultaneous high activity and selectivity is a promising strategy to increase energy supply and alleviate global warming.However,the absence of the active sites that is responsible for the adsorption and activation of CO_(2)and the generation of CO and H2via side reactions often lead to poor efficiency and low selectivity of the catalyst.Herein,Cu,Pd,and PdCu metal clusters cocatalyst-anchored defective TiO_(2)nanotubes(Cu/TiO_(2)-SBO,Pd/TiO_(2)-SBO,and Pd1Cu1/TiO_(2)-SBO)were designed via a simple solution impregnation reduction and applied for photocatalytic conversion of CO_(2)to CH_(4).The Pd1Cu1/TiO_(2)-SBO photocatalyst exhibits excellent catalytic performance among the other catalysts for photoreduction of CO_(2)into CH_(4).More interestingly,the product selectivity of CH_(4)reaches up to 100%with a rate of 25μmol g^(-1)h^(-1).In-situ diffuse reflectance infrared Fourier transform spectroscopy(DRIFTS)and density functional theory(DFT)simulations indicate that the main reasons for the high selectivity of CH_(4)are attributed to the PdCu alloy and oxygen vacancies,which jointly enhance the photoinduced carrier separation and lower energy barriers of key intermediates.Moreover,due to the tunable d-band center of the Cu site in the PdCu alloy,the generated intermediates can be well prevented from poisoning and promoted to participate in further reactions.Hopefully,the current study will provide insight into the development of new,highly selective photocatalysts for the visible light-catalytic reduction of CO_(2)into CH_(4).

关键词： PdCu alloy Defective TiO_(2) Photoreduction of CO_(2) Photocatalytic mechanism

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A study of novel real-time power balance strategy with virtual asynchronous machine control for regional integrated electric-thermal energy systems

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Science China Technological Sciences 2024年第7期67卷 2074-2086页

作者： WANG Rui li Ming-Jia WANG YiBo SUN qiuye ZHANG PinJia College of Information Science and Engineering Northeastern University School of Mechanical Engineering Beijing Institute of Technology Department of Electrical Engineering Tsinghua University

The development of regional integrated electric-thermal energy systems(RIETES) is considered a promising direction for modern energy supply systems. These systems provide a significant potential to enhance the comprehensive utilization and efficient management of energy resources. Therein, the real-time power balance between supply and demand has emerged as one pressing concern for system stability operation. However, current methods focus more on minute-level and hour-level power optimal scheduling methods applied in RIETES. To achieve real-time power balance, this paper proposes one virtual asynchronous machine(VAM) control using heat with large inertia and electricity with fast response speed. First, the coupling timescale model is developed that considers the dynamic response time scales of both electric and thermal energy systems. Second, a real-time power balance strategy based on VAM control can be adopted to the load power variation and enhance the dynamic frequency response. Then, an adaptive inertia control method based on temperature variation is proposed, and the unified expression is further established. In addition, the small-signal stability of the proposed control strategy is validated. Finally, the effectiveness of this control strategy is confirmed through MATLAB/Simulink and HIL(Hardware-in-the-Loop) experiments.

关键词： regional integrated electric-thermal energy systems real-time power balance virtual asynchronous machine adaptive inertia small-signal stability

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Structural design for electrocatalytic water splitting to realize industrial-scale deployment: Strategies, advances, and perspectives

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Journal of Energy Chemistry 2022年第7期31卷 129-153,I0004页

作者： Xianwei Fu Ruijuan Shi Shilong Jiao Mengmeng li qiuye li Engineering Research Center for Nanomaterials National&Local Joint Engineering Research Center for Applied Technology of Hybrid NanomaterialsHenan UniversityKaifeng 475004HenanChina Key Lab for Special Functional Materials of Ministry of Education Collaborative Innovation Center of Nano Functional Materials and ApplicationsHenan UniversityHenan UniversityKaifeng 475004HenanChina

The green hydrogen generation powered by renewable electricity promises the potential decarbonization of the hard-to-abate sector and is essential for the fulfillment of the Paris Agreement that attempts to limit the global average temperature rise in the range of 1.5–2.0 ℃ above the pre-industrial level by the end of this century. Tremendous efforts have been devoted to the optimization of the electrocatalytic performance of the catalysts under industrial-relevant current densities via rational structure design,which induces a preferential electron distribution that favors the adsorption/desorption behavior of the key intermediates, thus accelerating the reaction kinetics. In this review, a brief introduction of the current energy status will be first presented to necessitate the importance of green hydrogen.Followed by the basic concepts and fundamental understanding of the reaction mechanisms, we present efficient strategies for the enhancement of the electrocatalytic performance of the catalysts to meet the rigorous requirement under industrial conditions and the in-depth understanding behind the reinforcement will be briefly discussed next. Then the recent advances regarding the rational design of electrocatalysts operating at an industrial scale will be summarized. Finally, the challenges and perspectives in this thriving field will be proposed from our point of view.

关键词： Overall water splitting Industrial-scale current density Structural design Hydrogen evolution reaction Oxygen evolution reaction

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Development strategies and improved photocatalytic CO_(2) reduction performance of metal halide perovskite nanocrystals

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能源化学:英文版 2023年第8期83卷 397-422,I0011页

作者： Xianwei Fu Tingting Ren Shilong Jiao Zhihong Tian Jianjun Yang qiuye li Engineering Research Center for Nanomaterials National&Local Joint Engineering Research Center for Applied Technology of Hybrid NanomaterialsHenan UniversityKaifeng 475004HenanChina Key LabforSpecialFunctional Materials of Ministry of Education Collaborative Innovation Centerof NanoFunctional Materials and ApplicationsHenan UniversityKaifeng 475004 HenanChina Shenzhen Research Institute of Henan University Shenzhen 518000GuangdongChina

In recent years,photocatalytic CO_(2)reduction reaction(CRR) has attracted much scientific attention to overcome energy and environmental issues by converting CO_(2)into high-value-added chemicals utilizing solar energy.Metal halide perovskite(MHP) nanocrystals(NCs) are recognized as an ideal choice for CRR owing to their outstanding optoelectronic properties.Although great efforts have been devoted to designing more effective photocatalysts to optimize CRR performance,severe charge recombination,instability,and unsatisfactory activity have become major bottlenecks in developing perovskite-based photocatalysts.In this review,we mainly focus on the recent research progress in the areas of relevance.First,a brief insight into reaction mechanisms for CRR and structural features of MHPs are introduced.Second,efficient modification approaches for the improvement of the photocatalytic activity and stability of the perovskite-based catalysts are comprehensively reviewed.Third,the state-of-the-art achievements of perovskite-based photocatalysts for CRR are systematically summarized and discussed,which are focused on the modification approaches,structure design,and the mechanism of the CO_(2)reduction process.Lastly,the current challenges and future research perspectives in the design and application of perovskite materials are highlighted from our point of view to provide helpful insights for seeking breakthroughs in the field of CRR.This review may provide a guide for scientists interested in applying perovskite-based catalysts for solar-to-chemical energy conversion.

关键词： Photocatalytic CO_(2)reduction MHP nanocrystals Structure design Properties Stability

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Leaching kinetics of fluorine during the aluminum removal from spent li-ion battery cathode materials

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Journal of Environmental Sciences 2024年第4期138卷 312-325页

作者： Shengjie li Jianxin Zhu Research Center for Eco-Environmental Sciences Chinese Academy of SciencesBeijing 100085China University of Chinese Academy of Sciences Beijing 100049China

The high content of aluminum(Al)impurity in the recycled cathode powder seriously affects the extraction efficiency of Nickel,Cobalt,Manganese,and lithium resources and the actual commercial value of recycled materials,so Al removal is crucially important to conform to the industrial standard of spent li-ion battery cathode materials.In this work,we systematically investigated the leaching process and optimum conditions associated with Al removal from the cathode powder materials collected in a wet cathode-powder peeling and recycling production line of spent li-ion batteries(liBs).Moreover,we specifically studied the leaching of fluorine(F)synergistically happened along with the removal process of Al,which was not concerned about in other studies,but one of the key factors affecting pollution prevention in the recovery process.The mechanism of the whole process including the leaching of Al and F from the cathode powder was indicated by using NMR,FTIR,and XPS,and a defluoridation process was preliminarily investigated in this study.The leaching kinetics of Al could be successfully described by the shrinking core model,controlled by the diffusion process and the activation energy was 11.14 kJ/mol.While,the leaching of F was attributed to the dissolution of liPF6and decomposition of PVDF,and the kinetics associated was described by Avrami model.The interaction of Al and F is advantageous to realize the defluoridation to some degree.It is expected that our investigation will provide theoretical support for the large-scale recycling of spent liBs.

关键词： Al removal F leaching Cathode powder Heating alkali leaching Leaching kinetics

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Additives strategies to improving cycling stability of li metal batteries by modifying electrode electrolyte interphases

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Progress in Natural Science:Materials International 2024年第2期34卷 338-344页

作者： Yuan li Pengfei Huang Chunyu Cui Xiaoyuan Ma li Chen Zekun li linhai li Yuhong Tian School of Biological and Chemical Engineering Guangxi University of Science and Technology School of College of Chemistry and Chemical Engineering Hunan University Isky Future Energy Institute

li metal batteries（LMBs） have attracted much attention due to the ultra-high theoretical capacity of the li metal anode（LMA）.However,the uncontrollable dendrites growth and low coulombic efficiency hinder their practical application.Here,we explore 3,5-difluoropyridine（2F-BD） as a novel electrolyte additive to enable highperformance LMBs.The 2F-BD additive participates in and modifies the solvation structure of li ions by reducing the coordinated number of PF6-at the electrode surface,leading to the formation of a liF and li3N-rich solid electrolyte interphase（SEI）.The liF component increases the robustness of SEI and suppresses the formation of li dendrites,while the li3N component facilitates the transportation and reaction kinetics of li ions.As a result,the li‖li symmetric cell presents a stable cycling performance of up to 500 h at a current density of 1 mA cm-2.After coupling with liFePO4cathode,the obtained full cell achieves high specific capacities of 106.06 mA h g-1and 84.98 mA h g-1at 2.55 mA cm-2and 5.10 mA cm-2,respectively,and maintains a high capacity retention of84.0% after 1000 cycles at 0.13 mA cm-2,with an average cycling CE of 99.58%.

关键词： Electrolyte additive li dendrites li metal batteries liF and li3N-Rich electrode-electrolyte interphase liFePO4 cathode

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Highly-chlorinated inert and robust interphase without mineralization of oxide enhancing high-rate li metal batteries

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Chinese Chemical Letters 2024年第6期35卷 239-243页

作者： Long li Kang Yang Chenpeng Xi Mengchao li Borong li Gui Xu Yuanbin Xiao Xiancai Cui Zhiliang liu lingyun li Yan Yu Chengkai Yang Key Laboratory of Advanced Materials Technologies International(HongKong Macao and Taiwan)Joint Laboratory on Advanced Materials TechnologiesSchool of Materials Science and EngineeringFuzhou UniversityFuzhou 350108China College of Material Sciences and Chemical Engineering Harbin Engineering UniversityHarbin 150001China

Side reactions and dendrite growth triggered by the unstable interface and inhomogeneous deposition have become the biggest obstacle to the commercialization for lithium metal batteries.In this study,a highly-chlorinated organic-inorganic hybrid interfacial protective layer is developed by rationally tuning the interfacial passivation and robustness to achieve the convenient and efficient li metal anode.The polyvinyl chloride(PVC)can effectively resist water and oxygen,which is confirmed by density functional theory.The organic-dominant solid electrolyte interphases(SEI)with lithium chloride are investigated by the X-ray photoelectron spectroscopy(XPS)with little mineralization of oxide,such as li_(2)O and li_(2)CO_(3).With such artificial SEI,a uniform and dense lithium deposition morphology are formed and an ultra-long stable cycle of over 500 h are achieved even at an ultra-high current density of 10 m A/cm^(2).Moreover,the simple and convenient protected anode also exhibits excellent battery stability when paired with the liNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)and liFePO_(4)(LFP)cathode,showing great potential for the commercial application of lithium metal batteries.

关键词： Highly-chlorinated Water/oxygen resistance Stable interphase Dendrite-free lithium metal batteries High-rate

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Accelerating lithium-sulfur battery reaction kinetics and inducing 3D deposition of li2S using interactions between Fe3Se4 and lithium polysulfides

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Journal of Energy Chemistry 2024年第8期95卷 540-553页

作者： Yihan lin liheng li Longjie Tan Yongliang li Xiangzhong Ren Peixin Zhang Chuanxin He lingna Sun College of Chemistry and Environmental Engineering Shenzhen University

Although lithium-sulfur batteries（LSBs） exhibit high theoretical energy density,their practical application is hindered by poor conductivity of the sulfur cathode,the shuttle effect,and the irreversible deposition of li2S.To address these issues,a novel composite,using electrospinning technology,consisting of Fe3Se4and porous nitrogen-doped carbon nanofibers was designed for the interlayer of LSBs.The porous carbon nanofiber structure facilitates the transport of ions and electrons,while the Fe3Se4material adsorbs lithium polysulfides（liPSs） and accelerates its catalytic conversion process.Furthermore,the Fe3Se4material interacts with soluble liPSs to generate a new polysulfide intermediate,lixFeSycomplex,which changes the electrochemical reaction pathway and facilitates the three-dimensional deposition of li2S,enhancing the reversibility of LSBs.The designed LSB demonstrates a high specific capacity of1529.6 mA h g-1in the first cycle at 0.2 C.The rate performance is also excellent,maintaining an ultra-high specific capacity of 779.7 mA h g-1at a high rate of 8 C.This investigation explores the mechanism of the interaction between the interlayer and liPSs,and provides a new strategy to regulate the reaction kinetics and li2S deposition in LSBs.

关键词： Adsorption Catalysis Electrostatic spinning Interlayers li2S electrodeposition lithium-sulfur batteries Polysulfide intermediates

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Ultrathin organic solvent nanofiltration membrane with polydopamine-HKUST-1 interlayer for organic solvent separation

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Journal of Environmental Sciences 2024年第7期141卷 182-193页

作者： Haike li Xindong li Guozai Ouyang lijinhong Huang Lang li Wenhao li Wanfu Huang Duokun li Ganzhou Key Laboratory of Basin Pollution Simulation and Control Jiangxi University of Science and TechnologyGanzhou 341000China Innovation Center for Water Quality Security Technology at Ganjiang River Basin Jiangxi University of Science and TechnologyGanzhou 341000China School of Architecture and Design Jiangxi University of Science and TechnologyGanzhou 341000China WA School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityWA 6845Australia School of Materials Science and Engineering Tiangong UniversityTianjin 300387China

Polydopamine(PDA)and metal-organic skeleton HKUST-1 were co-deposited on the base membrane of hexamethylenediamine(HDA)-crosslinked polyetherimide(PEI)ultrafiltration membrane as the interlayer,and high-throughput organic solvent nanofiltration membrane(OSN)was prepared by interfacial polymerization and solvent activation reaction.The polyamide(PA)layer surface roughness from 28.4 nm in PA/PEI to 78.3 nm in PA/PDA-HKUST-10.6/PEI membrane,reduced the thickness of the separation layer from 79 to 14 nm,and significantly improved the hydrophilic,thermal and mechanical properties.The flux of the PA/PDA-HKUST-10.6/PEI membrane in a 0.1 g/L Congo Red(CR)ethanol solution at 0.6 MPa test pressure reached 21.8 L/(m^(2)·hr)and the rejection of CR was 92.8%.Solvent adsorption test,N,N-dimethylformamide(DMF)immersion experiment,and long-term operation test in ethanol showed that the membranes had high solvent tolerance.The solvent flux test demonstrated that,under the test pressure of 0.6 MPa,the flux of different solvents ranked as follows:methanol(56.9 L/(m^(2)·hr))>DMF(39.6 L/(m^(2)·hr))>ethanol(31.2 L/(m^(2)·hr))>IPA(4.5 L/(m^(2)·hr))>N-hexane(1.9 L/(m^(2)·hr)).The ability of the membranes to retain dyes in IPA/water dyes solution was also evaluated.The flux of the membrane was 30.4 L/(m^(2)·hr)and the rejection of CR was 91.6%when the IPA concentration reached 50%.This OSN membrane-making strategy is economical,environment-friendly and efficient,and has a great application prospect in organic solvent separation systems.

关键词： Interfacial polymerization Organic solvent nanofiltration Interlayer Metal-organic frameworks Polydopamine

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Boosting the performance of liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2) electrode by uniform li_(3)PO_(4) coating via atomic layer deposition

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Chinese Chemical Letters 2024年第5期35卷 499-503页

作者： Mingjiao Lu Zhixing Wang Gui Luo Huajun Guo Xinhai li Guochun Yan Qihou li Xianglin li Ding Wang Jiexi Wang School of Metallurgy and Environment Central South UniversityChangsha 410083China BASF ShanShan Battery Materials Co. Ltd.Changsha 410006China Engineering Research Center of the Ministry of Education for Advanced Battery Materials Central South UniversityChangsha 410083China Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy Central South UniversityChangsha 410083China School of Physics and Chemistry Hunan First Normal UniversityChangsha 410205China National and Local Joint Engineering Laboratory for lithium-ion Batteries and Materials Preparation Technology Key Laboratory of Advanced Battery Materials of Yunnan ProvinceFaculty of Metallurgical and Energy EngineeringKunming University of Science and TechnologyKunming 650093China

Ultra-high nickel material is considered to be a promising cathode material.However,with the increase of nickel content,the interfacial side reactions between the cathode and electrolyte become increasingly serious.Herein,an atomically controllable ionic conductor li_(3)PO_(4)(LPO)coating is deposited on the liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2)(NCM9064)based electrode by the atomic layer deposition method.The results shows that the LPO coating is uniformly and densely covered on the surface of secondary particles of NCM9064,helping to prevent the direct contact between the electrolyte and cathode during the chargingdischarging process.In addition,the coating layer is electrochemically stable.As a result,the interfacial side reactions during the long cycle are effectively suppressed,and the solid electrolyte interphase layer at the interface is stabilized.The electrode with 20 layers of LPO deposition(ALD-LPO-20)exhibits an excellent capacity retention of 81%after 200 cycles in 2.8-4.3 V at 25℃,which is 18%higher than the unmodified material(ALD-LPO-0).Besides,the moderate LPO coating improves the rate capability and high temperature cycling performance of NCM9064.This study provides a method for the modification of ultra-high nickel cathode materials and corresponding electrodes.

关键词： Ultra-high nickel material liNi_(0.90)Co_(0.06)Mn_(0.04)O_(2) Atomic layer deposition li_(3)PO_(4) Ionic conductor

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