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Incorporating empirical knowledge into data-driven variable selection for quantitative analysis of coal ash content by laser-induced breakdown spectroscopy

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Plasma Science and Technology 2024年第7期26卷 148-156页

作者：吕一涵宋惟然侯宗余王哲 State Key laboratory of Power System Operation and Control International Joint Laboratory on Low Carbon Clean Energy InnovationDepartment of Energy and Power EngineeringTsinghua UniversityBeijing 100084People’s Republic of China School of energy and Electrical Engineering Qinghai UniversityXining 810016People’s Republic of China Tsinghua University Shanxi Research Institute Clean EnergyTaiyuan 030032People’s Republic of China

Laser-induced breakdown spectroscopy(LIBS)has become a widely used atomic spectroscopic technique for rapid coal analysis.However,the vast amount of spectral information in LIBS contains signal uncertainty,which can affect its quantification performance.In this work,we propose a hybrid variable selection method to improve the performance of LIBS quantification.Important variables are first identified using Pearson's correlation coefficient,mutual information,least absolute shrinkage and selection operator(LASSO)and random forest,and then filtered and combined with empirical variables related to fingerprint elements of coal ash content.Subsequently,these variables are fed into a partial least squares regression(PLSR).Additionally,in some models,certain variables unrelated to ash content are removed manually to study the impact of variable deselection on model performance.The proposed hybrid strategy was tested on three LIBS datasets for quantitative analysis of coal ash content and compared with the corresponding data-driven baseline method.It is significantly better than the variable selection only method based on empirical knowledge and in most cases outperforms the baseline method.The results showed that on all three datasets the hybrid strategy for variable selection combining empirical knowledge and data-driven algorithms achieved the lowest root mean square error of prediction(RMSEP)values of 1.605,3.478 and 1.647,respectively,which were significantly lower than those obtained from multiple linear regression using only 12 empirical variables,which are 1.959,3.718 and 2.181,respectively.The LASSO-PLSR model with empirical support and 20 selected variables exhibited a significantly improved performance after variable deselection,with RMSEP values dropping from 1.635,3.962 and 1.647 to 1.483,3.086 and 1.567,respectively.Such results demonstrate that using empirical knowledge as a support for datadriven variable selection can be a viable approach to improve the accuracy and reliability of LIBS quantification.

关键词： laser-induced breakdown spectroscopy(LIBS) coal ash content quantitative analysis variable selection empirical knowledge partial least squares regression(PLSR)

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Surface iodine and pyrenyl-graphdiyne co-modified Bi catalysts for highly efficient CO_(2) electroreduction in acidic electrolyte

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Nano Research 2024年第4期17卷 2381-2387页

作者： Min Zhang Juan Wang Xin Rong Xiu-Li Lu Tong-Bu Lu MOE international joint laboratory of Materials Microstructure Institute for New Energy Materials and Low Carbon TechnologiesSchool of Materials Science and EngineeringTianjin University of TechnologyTianjin 300384China

CO_(2) electroreduction to formic acid/formate would contribute to alleviating the energy and climate crisis.This work reports a Bi-based catalyst derived from the in-situ electroreduction of Bi_(2)O_(2)CO_(3) modified with iodine and pyrenyl-graphdiyne(PGDY)on the surface for efficient electroreduction of CO_(2) in acidic electrolyte,with a high partial current density of 98.71 mA·cm^(-2) and high Faradaic efficiency(FE)>90%over the potential range from^(-1).2 to-1.5 V vs.reversible hydrogen electrode(RHE),as well as the long-term operational stability over 240 h without degradation in H-type cell.Experimental results and density function theory calculations show that the synergistic effect of surface iodine and PGDY is responsible for this active and extremely stable process of CO_(2) electroreduction via lowering the energy barriers for formation of*OCHO intermediate,suppressing the competitive HER by enhancing the concentration of both K+and CO_(2) at reaction interface,as well as preventing the dissolution and re-deposition of active Bi atoms on surface during catalytic reaction.This work provides new insight into designing highly active and stable electrocatalysts for CO_(2) reduction.

关键词： CO_(2) reduction electrocatalysis Bi-based catalysts acidic electrolyte

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Engineering Strategies for Suppressing the Shuttle Effect in Lithium–Sulfur Batteries

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Nano-Micro Letters 2024年第1期16卷 187-221页

作者： Jiayi Li Li Gao Fengying Pan Cheng Gong Limeng Sun Hong Gao Jinqiang Zhang Yufei Zhao Guoxiu Wang Hao Liu joint international laboratory On Environmental and energy Frontier Materials School of Environmental and Chemical EngineeringShanghai UniversityShanghaiPeople’s Republic of China Centre for clean energy Technology University of Technology SydneyBroadwaySydneyNSW 2007Australia

Lithium–sulfur(Li–S)batteries are supposed to be one of the most potential next-generation batteries owing to their high theoretical capacity and low cost.Nevertheless,the shuttle effect of firm multi-step two-electron reaction between sulfur and lithium in liquid electrolyte makes the capacity much smaller than the theoretical value.Many methods were proposed for inhibiting the shuttle effect of polysulfide,improving corresponding redox kinetics and enhancing the integral performance of Li–S batteries.Here,we will comprehensively and systematically summarize the strategies for inhibiting the shuttle effect from all components of Li–S batteries.First,the electrochemical principles/mechanism and origin of the shuttle effect are described in detail.Moreover,the efficient strategies,including boosting the sulfur conversion rate of sulfur,confining sulfur or lithium polysulfides(LPS)within cathode host,confining LPS in the shield layer,and preventing LPS from contacting the anode,will be discussed to suppress the shuttle effect.Then,recent advances in inhibition of shuttle effect in cathode,electrolyte,separator,and anode with the aforementioned strategies have been summarized to direct the further design of efficient materials for Li–S batteries.Finally,we present prospects for inhibition of the LPS shuttle and potential development directions in Li–S batteries.

关键词： Shuttle effect Designed strategies Li-S battery Lithium polysulfides

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Interface engineering strategy via electron-defect trimethyl borate additive toward 4.7 V ultrahigh-nickel LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)battery

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Journal of energy Chemistry 2024年第5期92卷 639-647页

作者： Yilin Zhang Yuqing Chen Qiu He Jinlong Ke Wei Wang Jian-Fang Wu Peng Gao Yanhua Li Jilei Liu College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan Province Key Laboratory for Advanced Carbon Materials and Applied TechnologyHunan UniversityChangsha 410082HunanChina College of Materials Science and Engineering Sichuan UniversityChengdu 610065SichuanChina School of Materials Science and Engineering Hunan Institute of TechnologyHengyang 421002HunanChina

The Li metal battery with ultrahigh-nickel cathode(LiNi_(x)M_(1-x)O_(2),M=Mn,Co,and x≥0.9)under high-voltage is regarded as one of the most promising approaches to fulfill the ambitious target of 400 Wh/kg.However,the practical application is impeded by the instability of electrode/electrolyte interface and Ni-rich cathode itself.Herein we proposed an electron-defect electrolyte additive trimethyl borate(TMB)which is paired with the commercial carbonate electrolyte to construct highly conductive fluorine-and boron-rich cathode electrolyte interface(CEI)on LiNi_(0.9)Co_(0.05)Mn_(0.05)O_(2)(NCM90)surface and solid electrolyte interphase(SEI)on lithium metal surface.The modified CEI effectively mitigates the structural transformation from layered to disordered rock-salt phase,and consequently alleviate the dissolution of transition metal ions(TMs)and its“cross-talk”effect,while the enhanced SEI enables stable lithium plating/striping and thus demonstrated good compatibility between electrolyte and lithium metal anode.As a result,the common electrolyte with 1 wt%TMB enables 4.7 V NCM90/Li cell cycle stably over 100 cycles with 70%capacity retention.This work highlights the significance of the electron-defect boron compounds for designing desirable interfacial chemistries to achieve high performance NCM90/Li battery under high voltage operation.

关键词： NCM90 batteries Electrolyte additive Trimethyl borate

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Heterostructured Pt-Ni_(3)Mo_(3)N formed via ammonia-containing polyoxometalates for highly efficient electrocatalytic hydrogen evolution in acid medium

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Journal of energy Chemistry 2024年第5期92卷 698-704页

作者： Bianqing Ren Xue Gong Jing Cao Dezheng Zhang Zizhun Wang Ping Song Ce Han Weilin Xu State Key laboratory of Electroanalytical Chemistry Jilin Province Key Laboratory of Low Carbon Chemical PowerChangchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied Chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina Key laboratory of Automobile Materials MOE School of Materials Science&EngineeringJilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy MaterialsElectron Microscopy Centerand International Center of Future ScienceJilin UniversityChangchun 130012JilinChina

Constructing heterostructured nanohybrid is considered as a prominent route to fabricate alternative electrocatalysts to commercial Pt/C for hydrogen evolution reaction(HER).In this work,(NH_(4))_(4)[NiH_(6)Mo_(6)O_(4)]·5H_(2)O polyoxometalates(NiMo_(6))are adopted as the cluster precursors for simple fabrication of heterostructured Pt-Ni_(3)Mo_(3)N nanohybrids supported by carbon black(Pt-Ni_(3)Mo_(3)N/C)without using additional N sources.The improved porosity and enhanced electronic interaction of Pt-Ni_(3)Mo_(3)N/C should be attributed to the integration of Pt with NiMo_(6),which favors the mass transport,promotes the formation of exposed catalytic sites,and benefits the regulation of intrinsic activity.Thus,the as-obtained Pt-Ni_(3)Mo_(3)N/C exhibits impressive and durable HER performance as indicated by the low overpotential of 13.7 mV at the current density of 10 mA cm^(-2) and the stable overpotential during continuous working at 100 mA cm^(-2) for 100 h.This work provides significant insights for the synthesis of new highly active heterostructured electrocatalysts for renewable energy devices.

关键词： Polyoxometalates Cluster precursors Heterostructured nanohybrids Hydrogen evolution reaction Electrocatalysis

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Optimizing high-coordination shell of Co-based single-atom catalysts for efficient ORR and zinc-air batteries

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Journal of energy Chemistry 2024年第8期95卷 306-314页

作者： Yugang Qi Qing Liang Kexin Song Xinyan Zhou Meiqi Liu Wenwen Li Fuxi Liu Zhou Jiang Xu Zou Zhongjun Chen Wei Zhang Weitao Zheng Key laboratory of Automobile Materials MOE School of Materials Science & Engineering Electron Microscopy Center and International Center of Future Science Jilin Provincial International Cooperation Key Laboratory of High-Efficiency Clean Energy Materials Jilin University Institute of High energy Physics Chinese Academy of Sciences

Atom-level modulation of the coordination environment for single-atom catalysts(SACs) is considered as an effective strategy for elevating the catalytic performance. For the MNxsite, breaking the symmetrical geometry and charge distribution by introducing relatively weak electronegative atoms into the first/second shell is an efficient way, but it remains challenging for elucidating the underlying mechanism of interaction. Herein, a practical strategy was reported to rationally design single cobalt atoms coordinated with both phosphorus and nitrogen atoms in a hierarchically porous carbon derived from metal-organic frameworks. X-ray absorption spectrum reveals that atomically dispersed Co sites are coordinated with four N atoms in the first shell and varying numbers of P atoms in the second shell(denoted as Co-N/P-C).The prepared catalyst exhibits excellent oxygen reduction reaction(ORR) activity as well as zinc-air battery performance. The introduction of P atoms in the Co-SACs weakens the interaction between Co and N,significantly promoting the adsorption process of *OOH, resulting in the acceleration of reaction kinetics and reduction of thermodynamic barrier, responsible for the increased intrinsic activity. Our discovery provides insights into an ultimate design of single-atom catalysts with adjustable electrocatalytic activities for efficient electrochemical energy conversion.

关键词： Electrocatalytic Oxygen reduction reaction Shell coordination optimization Single atom catalyst

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Recent advances and applications of single atom catalysts based electrochemical sensors

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Nano Research 2024年第4期17卷 2994-3013页

作者： Mingyue Wang Mingfu Ye Jieyue Wang Yong Xu Zhendong Wang Xinyue Tong Xinya Han Kui Zhang Wenhai Wang Konglin Wu Xianwen Wei Institute of clean energy and Advanced Nanocatalysis(iclean) School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China School of Materials Science and Engineering Anhui University of TechnologyMaanshan 243002China Anhui international Research Center of energy materials green manufacturing and biotechnology School of Chemistry and Chemical EngineeringAnhui University of TechnologyMaanshan 243002China carbon Cycle and Emission Control Research Center Low-Carbon Research InstituteAnhui University of TechnologyMaanshan 243002China

Single atom catalysts(SACs)have attracted considerable attention due to their unique structures and excellent catalytic performance,especially in the area of catalysis science and energy conversion and storage.In recent years,SACs have emerged as a new type of sensing material for constructing electrochemical sensors(ECSs),presenting excellent sensitivity,selectivity,and stability.Herein,we review the recent advances of SACs in electrochemical sensing and discuss the status quo of current SAC-based ECSs.Specifically,the fundamentals of SAC-based ECSs are outlined,including the involved central metal atoms and various supports of SACs in this field,the detection mechanisms,and improving strategies of SAC-based ECSs.Moreover,the important applications of SAC-based ECSs are listed and classified,covering the detection of reactive oxygen and nitrogen species,environmental pollutants,disease biomarkers,and pharmaceuticals.Last,based on abundant reported cases,the current conundrums of SAC-based ECSs are summarized,and the prediction of their future developing trends is also put forward.

关键词： single atom catalysts(SACs) electrochemical sensors(ECSs) reactive oxygen and nitrogen species environmental pollutants disease biomarkers pharmaceuticals

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A high Li-ion diffusion kinetics in multidimensional and compact-structured electrodes via vacuum filtration casting

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Journal of energy Chemistry 2024年第6期93卷 368-376,I0010页

作者： Jieqiong Li Ting Ouyang Lu Liu Shu Jiang Yongchao Huang M.-Sadeeq Balogun College of Materials Science and Engineering Hunan Joint International Laboratory of Advanced Materials and Technology for Clean EnergyHunan UniversityChangsha 410082HunanChina Institute of Environmental Research at Greater Bay Key Laboratory for Water Quality and Conservation of the Pearl River DeltaMinistry of EducationGuangzhou UniversityGuangzhou 510006GuangdongChina

Manufacturing process,diffusion co-efficient and areal capacity are the three main criteria for regulating thick electrodes for lithium-ion batteries(LIBs).However,simultaneously regulating these criteria for LIBs is desirable but remains a significant challenge.In this work,niobium pentoxide(Nb_(2)O_(5))anode and lithium iron phosphate(LiFePO_(4))cathode materials were chosen as the model materials and demonstrate that these three parameters can be simultaneously modulated by incorporation of micro-carbon fibers(MCF)and carbon nanotubes(CNT)with both Nb_(2)O_(5) and LFP via vacuum filtration approach.Both as-prepared MNC-20 anode and MLC-20 cathode achieves high reversible areal capacity of≈5.4 m A h cm^(-2)@0.1 C and outstanding Li-ion diffusion coefficients of≈10~(-8)cm~2 s~(-1)in the half-cell configuration.The assembled MNC-20‖MLC-20 full cell LIB delivers maximum energy and power densities of244.04 W h kg^(-1)and 108.86 W kg^(-1),respectively.The excellent electrochemical properties of the asprepared thick electrodes can be attributed to the highly conductive,mechanical compactness and multidimensional mutual effects of the MCF,CNT and active materials that facilitates rapid Li-ion diffusion kinetics.Furthermore,electrochemical impedance spectroscopy(EIS),symmetric cells analysis,and insitu Raman techniques clearly validates the enhanced Li-ion diffusion kinetics in the present architecture.

关键词： Thick electrodes carbon nanotubes Li-ion diffusion co-efficient Vacuum filtration technique High areal capacity Lithium-ion batteries

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Review on research and development of oxy-coal burner for carbon capture

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Science China(Technological Sciences) 2024年第3期67卷 647-672页

作者： GUO JunJun LIU JingZhang ZHANG Tai HU Fan LI PengFei LIU ZhaoHui ZHENG ChuGuang State Key laboratory of Coal Combustion School of Energy and Power EngineeringHuazhong University of Science and Technology Wuhan 430074China CCRC King Abdullah University of Science and Technology(KAUST)Thuwal 23955-6900Kingdom of Saudi Arabia Institute of Engineering Thermophysics Chinese Academy of SciencesBeijing 100049China University of Chinese Academy of Sciences Beijing 100049China National Key laboratory of High Efficiency and low carbon Utilization of Coal Beijing 100049China Institute of energy Research Jiangxi Academy of SciencesNanchang 330096China carbon Neutrality Research Center of Jiangxi Province Nanchang 330096China Faculty of Engineering China University of Geosciences(Wuhan)Wuhan 430074China National energy Research and Development Center of clean and low carbon Coal-based Power Generation Technologies Wuhan 430074China

In the past two decades, the oxy-fuel combustion of pulverized coal has been extensively developed, leading to the completion of several large industrial pilot oxy-fuel plants worldwide. Various types of oxy-fuel burners have been designed and tested in largescale pilot plants as key components of oxy-fuel combustion. These burners face major challenges in terms of their flame stability because of their decreasing stream momentum ratio and increasing carbon dioxide concentration. However, it offers flexibility in adjusting the oxygen concentration in each burner stream. This study aims to provide a comprehensive review of the state-of-the-art knowledge on oxy-coal burner design and operation in power plants. First, the combustion characteristics under oxy-fuel conditions are briefly introduced. Subsequently, the principal requirements and fundamental parameters of the oxy-coal burners are discussed. The development process of oxy-fuel burners is also presented. Moreover, a compatible design strategy and scaling-up techniques are described for oxy-coal burners developed by the authors over the past ten years. The performances of oxy-coal burners in three large pilot oxy-fuel plants worldwide are summarized and compared. Finally, concluding remarks are provided and potential research needs are suggested.

关键词： carbon capture oxy-fuel combustion oxy-fuel burner pulverized coal compatible design

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Design and modification of metal sulfide-based catalysts for lithiumsulfur batteries

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Particuology 2024年第3期86卷 86-100页

作者： Yufei Zhao Chuannan Geng Li Wang Haotian Yang Wei Lv Quan-Hong Yang Nanoyang Group State Key Laboratory of Chemical EngineeringSchool of Chemical Engineering and TechnologyNational Industry-Education Integration Platform of Energy Storageand Collaborative Innovation Center of Chemical Science and Engineering(Tianjin)Tianjin UniversityTianjin300072China Shenzhen Geim Graphene Center Engineering Laboratory for Functionalized Carbon MaterialsTsinghua Shenzhen International Graduate SchoolTsinghua UniversityShenzhen518055China Haihe laboratory of Sustainable Chemical Transformations Tianjin300192China joint School of National University of Singapore and Tianjin University International Campus of Tianjin UniversityFuzhou350207China

Metal sulfide(MS)have good conductivity,strong adsorption ability,and excellent catalytic activity for the conversion of sulfur species,and thus,show great promise as the catalysts in LieS batteries.However,the relationship between their properties and electrochemical performance is still unclear.Thus,further in-depth discussions are required to improve their design in Li-S batteries.This review systematically summarizes the basic structural and electrochemical properties of MSs and highlights the advantages that guarantee them as high-performance catalysts in Li-S batteries.Then,various modification strategies for MSs to enhance the catalytic activity,efficiency,and stability are also reviewed.At last,future opportunities for MS catalysts in Li-S batteries are proposed.

关键词： Lithium-sulfur battery Metal sulfide Catalysis

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