In this review,we primarily analyze the hydrogen production technologies based on water and biomass,including the economic,technological,and environmental impacts of different types of hydrogen production technologies...In this review,we primarily analyze the hydrogen production technologies based on water and biomass,including the economic,technological,and environmental impacts of different types of hydrogen production technologies based on these materials,and comprehensively compare them.Our analyses indicate that all renewable energy-based approaches for hydrogen production are more environmentally friendly than fossil-based hydrogen generation approaches.However,the technical ease and economic efficiency of hydrogen production from renewable sources of energy needs to be further improved in order to be applied on a large scale.Compared with other renewable energy-based methods,hydrogen production via biomass electrolysis has several advantages,including the ease of directly using raw biomass.Furthermore,its environmental impact is smaller than other approaches.Moreover,using a noble metal,catalyst-free anode for this approach can ensure a considerably low power consumption,which makes it a promising candidate for clean and efficient hydrogen production in the future.展开更多
Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbo...Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbon neutrality system that balances energy production and carbon reduction becomes crucial for the transformation of such basins.Under the framework of a green and intelligent energy system primarily based on“four news”,new energy,new electricity,new energy storage,and new intelligence,integrating a“super energy system”composed of a huge amount of underground resources of coal,oil,gas and heat highly overlapping with abundant wind and solar energy resources above ground,and a regional intelligent energy consumption system with coordinated development and utilization of fossil energy and new energy,with a carbon neutrality system centered around carbon cycling is essential.This paper aims to select the traditional oil and gas basins as“super energy basins”with the conditions to build world-class energy production and demonstration bases for carbon neutrality.The Ordos Basin has unique regional advantages,including abundant fossil fuel and new energy resources,as well as matching CO_(2)sources and sinks,position it as a carbon neutrality“super energy basin”which explores the path of transformation of traditional oil and gas basins.Under the integrated development concept and mode of“coal+oil+gas+new energy+carbon capture,utilization and storage(CCUS)/carbon capture and storage(CCS)”,the carbon neutrality in super energy basin is basically achieved,which enhance energy supply and contribute to the carbon peak and carbon neutrality goals,establish a modern energy industry and promote regional green and sustainable development.The pioneering construction of the world-class carbon neutrality“super energy system”demonstration basin in China represented by the Ordos Basin will reshape the new concept and new mode of exploration and development of super energy basins,which is of great significance to the global energy revolution under carbon neutrality.展开更多
Under global consensus on carbon neutrality and the intensification of regional conflicts,new energy has become the primary direction for various countries to achieve energy security and green development.Represented ...Under global consensus on carbon neutrality and the intensification of regional conflicts,new energy has become the primary direction for various countries to achieve energy security and green development.Represented by wind,solar,geothermal,hydrogen and stored energy,and controllable nuclear fusion,the technological and scale advantages of new energy are being continuously strengthened.Low-cost wind,solar,and stored energy will support the global energy transition.The production and utilization of new energy enter a rapid development phase.In 2022,the average global consumption of new energy accounted for 18.2%,and it is expected to reach around 55%by 2050.The distribution of the world's energy resources,consumption regions,technological development,per capita consumption,energy-saving fields,and carbon emissions is uneven.The acceleration of low-carbon development in fossil fuels,the scale-up of renewable energy,and the intelligentization of energy management drives the rapid transition of global energy.展开更多
Chinese-style modernization emphasizes the harmonious coexistence of man and nature and actively yet prudently promotes carbon peak and carbon neutrality.It delves deeply into the energy revolution,upholding the follo...Chinese-style modernization emphasizes the harmonious coexistence of man and nature and actively yet prudently promotes carbon peak and carbon neutrality.It delves deeply into the energy revolution,upholding the following principles:the“independence”of energy production,the“green”energy supply,the“security”of energy reserves,the“efficiency”of energy consumption,the“intelligence”of energy management,and the“economy”of energy costs.Efforts are being made to accelerate the planning and construction of a new type of energy system that is green and smart,with new energy,new electricity,new stored energy,and new smart energy as the mainstays,to ensure energy security.Currently,China is an energy power but not an energy superpower,and its energy consumption structure still needs further optimization.China’s new energy security strategy is composed of energy consumption revolution,energy supply revolution,energy technology revolution,and energy system revolution,complemented by comprehensive strengthening of international cooperation.This approach is aimed at advancing China’s energy revolution and transforming the nation’s energy supply pattern and shifting from a consumption mix in 2022.展开更多
We present a simple and reliable method,based on the over-barrier model and Lindhard’s formula,to calculate the energy loss,charge transfer,and normalized intensity of highly charged ions penetrating through 2D ultra...We present a simple and reliable method,based on the over-barrier model and Lindhard’s formula,to calculate the energy loss,charge transfer,and normalized intensity of highly charged ions penetrating through 2D ultrathin materials,including graphene and carbon nanomembranes.According to our results,the interaction between the ions and the 2D material can be simplified as an equivalent two-body collision,and we find that full consideration of the charge exchange effect is key to understanding the mechanism of ion energy deposition in an ultrathin target.Not only can this semiclassical model be used to evaluate the ion irradiation effect to a very good level of accuracy,but it also provides important guidance for tailoring the properties of 2D materials using ion beams.展开更多
Unconventional oil and gas resources are closely to the retaining ability of hydrocarbon of source rock. The detained hydrocarbon can be divided to two parties: organic retaining ability including the swelling and ad...Unconventional oil and gas resources are closely to the retaining ability of hydrocarbon of source rock. The detained hydrocarbon can be divided to two parties: organic retaining ability including the swelling and adsorption function of kerogen and retaining ability of organic pore, and inorganic retaining ability including adsorption of detrital minerals and retaining ability of inorganic pore.展开更多
For the performance optimization strategies of hard carbon,heteroatom doping is an effective way to enhance the intrinsic transfer properties of sodium ions and electrons for accelerating the reaction kinetics.However...For the performance optimization strategies of hard carbon,heteroatom doping is an effective way to enhance the intrinsic transfer properties of sodium ions and electrons for accelerating the reaction kinetics.However,the previous work focuses mainly on the intrinsic physicochemical property changes of the material,but little attention has been paid to the resulting interfacial regulation of the electrode surface,namely the formation of solid electrolyte interphase(SEI)film.In this work,element F,which has the highest electronegativity,was chosen as the doping source to,more effectively,tune the electronic structure of the hard carbon.The effect of F-doping on the physicochemical properties of hard carbon was not only systematically analyzed but also investigated with spectroscopy,optics,and in situ characterization techniques to further verify that appropriate F-doping plays a positive role in constructing a homogenous and inorganic-rich SEI film.The experimentally demonstrated link between the electronic structure of the electrode and the SEI film properties can reframe the doping optimization strategy as well as provide a new idea for the design of electrode materials with low reduction kinetics to the electrolyte.As a result,the optimized sample with the appropriate F-doping content exhibits the best electrochemical performance with high capacity(434.53 mA h g^(-1)at 20mA g^(-1))and excellent rate capability(141 mAh g^(-1)at 400 mA g^(-1)).展开更多
In the mid-21st century,natural gas will enter its golden age,and the era of natural gas is arriving.This paper reviews the development stages of global natural gas industry and the enlightenment of American shale gas...In the mid-21st century,natural gas will enter its golden age,and the era of natural gas is arriving.This paper reviews the development stages of global natural gas industry and the enlightenment of American shale gas revolution,summarizes the development history and achievements of the natural gas industry in China,analyzes the status and challenges of natural gas in the green and low-carbon energy transition,and puts forward the natural gas industry development strategies under carbon neutral target in China.The natural gas industry in China has experienced three periods:start,growth,and leap forward.At present,China has become the fourth largest natural gas producer and third largest natural gas consumer in the world,and has made great achievements in natural gas exploration and development theory and technology,providing important support for the growth of production and reserves.China has set its goal of carbon neutrality to promote green and sustainable development,which brings opportunities and challenges for natural gas industry.Natural gas has significant low-carbon advantages,and gas-electric peak shaving boosts new energy development;the difficulty and cost of development are more prominent.For the national energy security and harmonious development between economy and ecology under the carbon neutral goal,based on the principle of"comprehensive planning,technological innovation,multi-energy complementarity,diversified integration,flexibility and efficiency,optimization and upgrading",the construction of the production-supplystorage-marketing system has to be improved so as to boost the development of the natural gas industry.First,it is necessary to strengthen efforts in the exploration and development of natural gas,making projects and arrangement in key exploration and development areas,meanwhile,it is urgent to make breakthroughs in key science theories and technologies,so as to increase reserve and production.Second,it should promote green and innovative development of the natural gas by developing new techniques,expanding new fields and integrating with new energy.Third,there is a demand to realize transformation and upgrading of the supply and demand structure of natural gas by strengthening the layout of pipeline gas,liquefied natural gas and the construction of underground gas storage,establishing reserve system for improving abilities of emergency response and adjustment,raising the proportion of natural gas in the primary energy consumption and contributing to the transformation of energy consumption structure,realizing low-carbon resources utilization and clean energy consumption.展开更多
Investigating the formation mechanisms of carbonate geothermal reservoirs is of theoretical and practical significance for summarizing the formation pattern of geothermal resources and further guiding their effective ...Investigating the formation mechanisms of carbonate geothermal reservoirs is of theoretical and practical significance for summarizing the formation pattern of geothermal resources and further guiding their effective exploitation.The Beijing-Tianjin-Hebei Plain(BTHP),predominantly located within the Jizhong Depression and Cangxian Uplift in the Bohai Bay Basin,serves as the primary region for geothermal exploitation and utilization in China.More than 1500 geothermal wells have been drilled therein,with water temperature at the wellhead ranging from 55 to 110°C,single-well flow rate ranging between 80 and 120 m^(3)/h,and cumulative heating area exceeding 100×10^(6)m^(3).However,the exploration and research in the region remain limited overall.As per the previous geothermal and petroleum exploration results and the latest geothermal drilling data,this study comprehensively evaluated the geothermal resources of karst geothermal reservoirs.The results show that two suites of carbonate karst reservoirs,namely the Jxw Formation and the Ordovician strata,have primarily developed in the BTHP,and their formation and evolution can be divided into four stages:the Mesoproterozoic-Early Paleozoic stage with carbonate sedimentation and the development of interlayer karst,the Late Paleozoic stage with the development of direct sedimentary cover,the Mesozoic stage with compressional uplifting and development of buried hill karst,and the Cenozoic stage with regional cover deposition and the modification and finalization of karst geothermal reservoirs.Accordingly,the porosity evolution history of the geothermal reservoirs is composed of three stages,namely a significant decrease followed by a minor increase,a gradual decline,and then a small fluctuation from increase to decrease before slowly rising again.The karstification in geothermal reservoirs can be summarized into quasi-syngenetic karstification,epigenetic karstification,and burial karstification,which can be subdivided into seven subcategories.The carbonate geothermal reservoirs in the study area boast total geothermal resources of 53.821×10^(9)GJ,or 184.155×10^(9)t of standard coal equivalent(tce),and the annual exploitable geothermal resources in the urban area can heat an area of(400‒500)×10^(6)m^(3),indicating great potential of geothermal exploitation.展开更多
Regulating the catalyst electronic structure is critical for improving the adsorption and catalytic conversion of lithium polysulfides(LiPSs)in lithium-sulfur batteries(Li-S),yet which has been overlooked in current s...Regulating the catalyst electronic structure is critical for improving the adsorption and catalytic conversion of lithium polysulfides(LiPSs)in lithium-sulfur batteries(Li-S),yet which has been overlooked in current studies.In this work,structurally defined Ag_(30)Pd_(4)nanoclusters were loaded onto reduced graphene oxide(Ag_(30)Pd_(4)/rGO)as a modification material for polypropylene(PP)separators to elucidate the catalytic activity towards lithium polysulfides and the impact on the electrochemical properties to lithium sulfur batteries.This unique d-πcombination promotes charge transfer,influences overall charge states,and further enhances adsorption energies in potential reaction pathways with lithium polysulfides.Consequently,the Ag_(30)Pd_(4)/rGO/PP modified batteries exhibited an exceptionally low-capacity decay rate of 0.026%per cycle at 1.0C over 1000 stable cycles and 9.75 mAh cm^(-2)excellent performance even with lean electrolyte and high sulfur loading(9.7 mg cm^(-2)).This study paves a path for employing ultrasmall bimetallic nanoclusters to promote the polysulfides redox kinetics hence boosting the lithiumsulfur battery performance.展开更多
The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular surfactants.However,the mechanism behind it remains elusive and deba...The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular surfactants.However,the mechanism behind it remains elusive and debatable.Herein,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalocyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO_(2) and CO_(2)RR intermediates were explored by density functional theory(DFT)calculations.It was found that the selectivity and activity of CO_(2)RR towards C_(2)products on Cu NWs were considerably enhanced from 35.2%to 69.9%by surface decoration of CoPc.DFT calculations revealed that CO_(2)RR can proceed in the interphase between Cu substrate and CoPc,and the CO_(2)RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO_(2),CO and CO_(2)RR intermediates,thus reducing the free energy for CO-COcoupling towards C_(2)products.The synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker synergistic interaction of COintermediates with MPc and Cu substrate and only a slight enhancement of CO_(2)RR towards C_(2) products were observed.This study demonstrates a synergistic catalysis pathway for CO_(2)RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO_(2)RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.展开更多
Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels h...Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels have drawn a considerable amount of attention but most of them operate in alkali solutions.However,the frequently studied Co-Fe spinel system never exhibits appreciable stability in nonbasic conditions,not to mention attract further investigation on its key structural motif and transition states for activity loss.Herein,we report exceptional stable Co-Fe spinel oxygen evolution catalysts(~30%Fe is optimal)in a neutral electrolyte,owing to its unique metal ion arrangements in the crystal lattice.The introduced iron content enters both the octahedral and tetrahedral sites of the spinel as Fe^(2+)and Fe^(3+)(with Co ions having mixed distribution as well).Combining density functional theory calculations,we find that the introduction of Fe to Co_(3)O_(4)lowers the covalency of metal-oxygen bonds and can help suppress the oxidation of Co^(2+/3+)and 0^(2-).It implies that the Co-Fe spinel will have minor surface reconstruction and less lattice oxygen loss during the oxygen evolution reaction process in comparison with Co_(3)O_(4)and hence show much better stability.These findings suggest that there is still much chance for the spinel structures,especially using reasonable sublattices engineering via multimetal doping to develop advanced oxygen evolution catalysts.展开更多
The alkaline hydrogen evolution reaction(HER) on Pt-based catalysts is largely limited by the slow water dissociation kinetics. Pt-based single atom alloy catalysts(SAAC) with water dissociation sites have been demons...The alkaline hydrogen evolution reaction(HER) on Pt-based catalysts is largely limited by the slow water dissociation kinetics. Pt-based single atom alloy catalysts(SAAC) with water dissociation sites have been demonstrated as excellent alkaline HER catalysts. However, the regulation of their activity and stability at the atomic scale is still a great challenge. Herein, the kinetic and stability issues are successfully resolved via engineering the electronic structure of Pt-Co SAAC by Au-induced tensile strain. The atomic dispersion of Co into the Pt shell was confirmed by extended X-ray absorption fine structure and the electronic structure and catalytic HER performance was modulated by the tensile strain induced by the Pt shell thickness. An inverse volcano-type relation between HER activity and surface strain was found.Density functional theory(DFT) calculations reveal that the Au-induced tensile strain on Pt-Co shell can not only boost the adsorption and dissociation kinetics of water at Co site by upshifting the dband and promoting the electron transfer, but also downshift the d-band center of Pt in Pt-Co shell, leading to optimized H* adsorption/desorption. The champion catalyst provides an overpotential of only 14 m V at the current density of 10 mA cm^(-2). This work not only provides an effective strategy for the construction of single-atom alloy electrocatalysts for high performance toward alkaline HER but also sheds light on the understanding of the reaction mechanism at the atomic level.展开更多
The carbon content of bituminous coal samples was analyzed by laser-induced breakdown spectroscopy. The 266 nm laser radiation was utilized for laser ablation and plasma generation in air. The partial least square met...The carbon content of bituminous coal samples was analyzed by laser-induced breakdown spectroscopy. The 266 nm laser radiation was utilized for laser ablation and plasma generation in air. The partial least square method and the dominant factor bused PLS method were used to improve the measurement accuracy of the carbon content of coal. The results showed that the PLS model could achieve good measurement accuracy, and the dominant factor based PLS model could further improve the measurement accuracy. The coefficient of determination and the root-mean-square error of prediction of the PLS model were 0.97 and 2.19%, respectively; and those values for the dominant factor based PLS model were 0.99 and 1.51%, respectively. The results demonstrated that the 266 nm wavelength could accurately measure the carbon content of bituminous coal.展开更多
The slow redox dynamics and dissolution of polysulfides in lithium-sulfur(Li-S)batteries result in poor rate performance and rapid decay of battery capacity,thus limiting their practical application.Ferroelectric bari...The slow redox dynamics and dissolution of polysulfides in lithium-sulfur(Li-S)batteries result in poor rate performance and rapid decay of battery capacity,thus limiting their practical application.Ferroelectric barium titanate(BT)nanoparticles have been reported to effectively improve the electrochemical performance of Li-S batteries due to the inherent self-polarization and high adsorption capacity of the BT nanoparticles towards polysulfides.Here in this paper,BT nanoparticles,behave as highly efficient electrocatalyst and demonstrate much higher redox dynamics towards the conversion reaction of polysulfides and Li2S than TiO2,as shown by both electrochemical measurements and density functional theory calculation.The coupling of the sulfur host of the hollow and graphitic carbon flakes(HGCF)and the BT nanoparticles(HGCF/S-BT)enable excellent electrochemical performance of Li-S batteries,delivering a0.047%capacity decay per cycle in 1000 cycles at 1 C,788 mAh g^-1 at 2 C and a reversible capacity of613 mAh g^-1 after 300 cycles at a current density of 0.5 C at a S loading of 3.4 mg cm^-2.HGCF/S-BT also shows great promise for practical application in flexible devices as demonstrated on the soft-packaged Li-S batteries.展开更多
Laser-induced breakdown spectroscopy(LIBS) is a potential technology for online coal property analysis,but successful quantitative measurement of calorific value using LIBS suffers from relatively low accuracy caused ...Laser-induced breakdown spectroscopy(LIBS) is a potential technology for online coal property analysis,but successful quantitative measurement of calorific value using LIBS suffers from relatively low accuracy caused by the matrix effect.To solve this problem,the support vector machine(SVM) and the partial least square(PLS) were combined to increase the measurement accuracy of calorific value in this study.The combination model utilized SVM to classify coal samples into two groups according to their volatile matter contents to reduce the matrix effect,and then applied PLS to establish calibration models for each sample group respectively.The proposed model was applied to the measurement of calorific values of 53 coal samples,showing that the proposed model could greatly increase accuracy of the measurement of calorific values.Compared with the traditional PLS method,the coefficient of determination(R2) was improved from 0.93 to 0.97,the root-mean-square error of prediction was reduced from 1.68 MJ kg-1 to1.08 MJ kg-1,and the average relative error was decreased from 6.7% to 3.93%,showing an overall improvement.展开更多
1.Introduction Climate change is one of the most severe challenges facing the world today.At present,China produces total annual carbon dioxide(CO_(2))emissions of over 10 billion tonnes,topping the world in this rega...1.Introduction Climate change is one of the most severe challenges facing the world today.At present,China produces total annual carbon dioxide(CO_(2))emissions of over 10 billion tonnes,topping the world in this regard.Although coal empowers China’s economic development,its use presents a great challenge to the nation’s desired goals of peaking carbon emissions and achieving carbon neutrality.In this context,the low-carbon utilization of coal is an inevitable trend for future development.Exploring new ways to reduce CO_(2) emissions on a large scale in the utilization of coal—especially during coal-fired power generation—is essential in order for China to achieve carbon neutrality.展开更多
Carbon dioxide storage and utilization has become an inevitable trend and choice for sustainable development under the background of global climate change and carbon neutrality.Carbon industry which is dominated by CO...Carbon dioxide storage and utilization has become an inevitable trend and choice for sustainable development under the background of global climate change and carbon neutrality.Carbon industry which is dominated by CO_(2) capture,utilization and storage/CO_(2) capture and storage(CCUS/CCS)is becoming a new strategic industry under the goal of carbon neutrality.The sustainable development of carbon industry needs to learn from the experiences of global oil and gas industry development.There are three types of“carbon”in the earth system.Black carbon is the CO_(2) that has not been sequestered or used and remains in the atmosphere for a long time;grey carbon is the CO_(2) that has been fixed or permanently sequestered in the geological body,and blue carbon is the CO_(2) that could be converted into products for human use through biological,physical,chemical and other ways.The carbon industry system covers carbon generation,carbon capture,carbon transportation,carbon utilization,carbon sequestration,carbon products,carbon finance,and other businesses.It is a revolutionary industrial field to completely eliminate“black carbon”.The development of carbon industry technical system takes carbon emission reduction,zero carbon,negative carbon and carbon economy as the connotation,and the construction of a low-cost and energy-efficient carbon industry system based on CCUS/CCS are strategic measures to achieve the goal of carbon neutrality and clean energy utilization globally.This will promote the“four 80%s”transformation of China's energy supply,namely,to 2060,the percentage of zero-carbon new energy in the energy consumption will be over 80%and the CO_(2) emission will be decreased by 80%to ensure the carbon emission reduction of total 80×10^(8) t from the percentage of carbon-based fossil energy in the energy consumption of over 80%,and the percentage of CO_(2) emission from energy of over 80%in 2021.The carbon industry in China is facing three challenges,large CO_(2) emissions,high percentage of coal in energy consumption,and poor innovative system.Three strategic measures are proposed accordingly,including:(1)unswervingly develop carbon industrial system and ensure the achievement of carbon neutrality as scheduled by 2060;(2)vigorously develop new energy sources and promote a revolutionary transformation of China’s energy production and consumption structure;(3)accelerate the establishment of scientific and technological innovation system of the whole CO_(2) industry.It is of great significance for continuously optimization of ecological environment and construction of green earth and ecological earth to develop the carbon industry system,utilize clean energy,and achieve the strategic goal of global carbon neutrality.展开更多
Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nick...Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nickel-rich cathode materials is one of the major barriers for the large-scale usage of LIBs.The existing obstructions that suppress the capacity degradation of nickel-rich cathode materials are as a result of phase transition,mechanical instability,intergranular cracks,side reaction,oxygen loss,and thermal instability during cycling.Core–shell structures,oxidating precursors,electrolyte additives,doping/coating and synthesizing single crystals have been identified as effective methods to improve cycling stability of nickel-rich cathode materials.Herein,recent progress of surface modification,e.g.coating and doping,in nickel-rich cathode materials are summarized based on Periodic table to provide a clear understanding.Electrochemical performances and mechanisms of modified structure are discussed in detail.It is hoped that an overview of synthesis and surface modification can be presented and a perspective of nickel-rich materials in LIBs can be given.展开更多
The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S ba...The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S batteries is demonstrated to be an effective strategy to overcome this problem.Herein,cobalt nanoparticles confined in nitrogen co-doped porous carbon framework(Co-CN)were developed from pyrolysis of ZIF-67 and used as interlayer of PP separator for Li-S batteries,and were functionalized by four pyrrole derivatives,1-phenylpyrrole,1-methyl pyrrole,1-(p-toluenesulfonyl)pyrrole,and 1-pyrrole,respectively,which were screened in terms of the electron-withdrawing/donating ability of the substituent groups on the pyrrolic nitrogen.The impact of the molecular structure of pyrrole derivatives on the interaction with Li PSs and the electrochemical performance of Li-S batteries were explored by nuclear magnetic resonance and theoretical calculation.It is uncovered that 1-phenylpyrrole shows the highest enhancement of redox kinetics of Li PSs,attributing to the optimal interaction with Co nanoparticles and Li PSs.Therefore,1-phenylpyrrole modified Co-CN interlayer enables the best electrochemical performance for the Li-S batteries,delivering a specific capacity of 562 m Ah g^(-1)at 5 C and a capacity of 538,526,and 449 m Ah g^(-1)after 500 cycles at 1,2,and 3 C,respectively.At a high sulfur loading of 5.5 mg cm^(-2),it achieves a capacity of 440 m Ah g^(-1)after 500 cycles at 1 C.This work reveals the interaction mechanism among Li PSs,Co nanoparticles and the molecular modifiers in improving the electrochemical performance of Li-S batteries.展开更多
基金supported by the Beijing Science and Technology Major Project (Grant No.Z171100002017021)CHN Energy Science and Technology Innovation Project (2017B1BE00100)
文摘In this review,we primarily analyze the hydrogen production technologies based on water and biomass,including the economic,technological,and environmental impacts of different types of hydrogen production technologies based on these materials,and comprehensively compare them.Our analyses indicate that all renewable energy-based approaches for hydrogen production are more environmentally friendly than fossil-based hydrogen generation approaches.However,the technical ease and economic efficiency of hydrogen production from renewable sources of energy needs to be further improved in order to be applied on a large scale.Compared with other renewable energy-based methods,hydrogen production via biomass electrolysis has several advantages,including the ease of directly using raw biomass.Furthermore,its environmental impact is smaller than other approaches.Moreover,using a noble metal,catalyst-free anode for this approach can ensure a considerably low power consumption,which makes it a promising candidate for clean and efficient hydrogen production in the future.
基金Supported by the National Natural Science Foundation of China(42072187)PetroChina Science and Technology Special Project(2021ZZ01-05)。
文摘Super oil and gas basins provide the energy foundation for social progress and human development.In the context of climate change and carbon peak and carbon neutrality goals,constructing an integrated energy and carbon neutrality system that balances energy production and carbon reduction becomes crucial for the transformation of such basins.Under the framework of a green and intelligent energy system primarily based on“four news”,new energy,new electricity,new energy storage,and new intelligence,integrating a“super energy system”composed of a huge amount of underground resources of coal,oil,gas and heat highly overlapping with abundant wind and solar energy resources above ground,and a regional intelligent energy consumption system with coordinated development and utilization of fossil energy and new energy,with a carbon neutrality system centered around carbon cycling is essential.This paper aims to select the traditional oil and gas basins as“super energy basins”with the conditions to build world-class energy production and demonstration bases for carbon neutrality.The Ordos Basin has unique regional advantages,including abundant fossil fuel and new energy resources,as well as matching CO_(2)sources and sinks,position it as a carbon neutrality“super energy basin”which explores the path of transformation of traditional oil and gas basins.Under the integrated development concept and mode of“coal+oil+gas+new energy+carbon capture,utilization and storage(CCUS)/carbon capture and storage(CCS)”,the carbon neutrality in super energy basin is basically achieved,which enhance energy supply and contribute to the carbon peak and carbon neutrality goals,establish a modern energy industry and promote regional green and sustainable development.The pioneering construction of the world-class carbon neutrality“super energy system”demonstration basin in China represented by the Ordos Basin will reshape the new concept and new mode of exploration and development of super energy basins,which is of great significance to the global energy revolution under carbon neutrality.
基金"Study on the Pore Preservation Mechanism during CO_(2) Enhanced Oil Recovery in Continental Tight Sandstone"funded by the National Natural Science Foundation of China (Project No.:42072187)Topic 5"Research on Key Technologies for Evaluation and Monitoring of CCUS/CCS Geological Storage Site Selection"of CNPC Major Science and Technology Special Project"Study on the Pore Preservation Mechanism during the CO_(2) Enhanced Oil Recovery in Continental Tight Sandstone"(Project No.:2021ZZ01-05)
文摘Under global consensus on carbon neutrality and the intensification of regional conflicts,new energy has become the primary direction for various countries to achieve energy security and green development.Represented by wind,solar,geothermal,hydrogen and stored energy,and controllable nuclear fusion,the technological and scale advantages of new energy are being continuously strengthened.Low-cost wind,solar,and stored energy will support the global energy transition.The production and utilization of new energy enter a rapid development phase.In 2022,the average global consumption of new energy accounted for 18.2%,and it is expected to reach around 55%by 2050.The distribution of the world's energy resources,consumption regions,technological development,per capita consumption,energy-saving fields,and carbon emissions is uneven.The acceleration of low-carbon development in fossil fuels,the scale-up of renewable energy,and the intelligentization of energy management drives the rapid transition of global energy.
文摘Chinese-style modernization emphasizes the harmonious coexistence of man and nature and actively yet prudently promotes carbon peak and carbon neutrality.It delves deeply into the energy revolution,upholding the following principles:the“independence”of energy production,the“green”energy supply,the“security”of energy reserves,the“efficiency”of energy consumption,the“intelligence”of energy management,and the“economy”of energy costs.Efforts are being made to accelerate the planning and construction of a new type of energy system that is green and smart,with new energy,new electricity,new stored energy,and new smart energy as the mainstays,to ensure energy security.Currently,China is an energy power but not an energy superpower,and its energy consumption structure still needs further optimization.China’s new energy security strategy is composed of energy consumption revolution,energy supply revolution,energy technology revolution,and energy system revolution,complemented by comprehensive strengthening of international cooperation.This approach is aimed at advancing China’s energy revolution and transforming the nation’s energy supply pattern and shifting from a consumption mix in 2022.
基金supported by the NSFC(Grant No.11705010)the NSAF(Grant No.U1230111),the IAEA(CRP No.F11020 and Contract No.21063)the China Postdoctoral Science Foundation(Grant No.2019M650351)。
文摘We present a simple and reliable method,based on the over-barrier model and Lindhard’s formula,to calculate the energy loss,charge transfer,and normalized intensity of highly charged ions penetrating through 2D ultrathin materials,including graphene and carbon nanomembranes.According to our results,the interaction between the ions and the 2D material can be simplified as an equivalent two-body collision,and we find that full consideration of the charge exchange effect is key to understanding the mechanism of ion energy deposition in an ultrathin target.Not only can this semiclassical model be used to evaluate the ion irradiation effect to a very good level of accuracy,but it also provides important guidance for tailoring the properties of 2D materials using ion beams.
文摘Unconventional oil and gas resources are closely to the retaining ability of hydrocarbon of source rock. The detained hydrocarbon can be divided to two parties: organic retaining ability including the swelling and adsorption function of kerogen and retaining ability of organic pore, and inorganic retaining ability including adsorption of detrital minerals and retaining ability of inorganic pore.
基金National Key R&D Program of China,Grant/Award Number:2022YFB4000120Fundamental Research Funds for the Central Universities,Grant/Award Number:2022ZYGXZR101。
文摘For the performance optimization strategies of hard carbon,heteroatom doping is an effective way to enhance the intrinsic transfer properties of sodium ions and electrons for accelerating the reaction kinetics.However,the previous work focuses mainly on the intrinsic physicochemical property changes of the material,but little attention has been paid to the resulting interfacial regulation of the electrode surface,namely the formation of solid electrolyte interphase(SEI)film.In this work,element F,which has the highest electronegativity,was chosen as the doping source to,more effectively,tune the electronic structure of the hard carbon.The effect of F-doping on the physicochemical properties of hard carbon was not only systematically analyzed but also investigated with spectroscopy,optics,and in situ characterization techniques to further verify that appropriate F-doping plays a positive role in constructing a homogenous and inorganic-rich SEI film.The experimentally demonstrated link between the electronic structure of the electrode and the SEI film properties can reframe the doping optimization strategy as well as provide a new idea for the design of electrode materials with low reduction kinetics to the electrolyte.As a result,the optimized sample with the appropriate F-doping content exhibits the best electrochemical performance with high capacity(434.53 mA h g^(-1)at 20mA g^(-1))and excellent rate capability(141 mAh g^(-1)at 400 mA g^(-1)).
文摘In the mid-21st century,natural gas will enter its golden age,and the era of natural gas is arriving.This paper reviews the development stages of global natural gas industry and the enlightenment of American shale gas revolution,summarizes the development history and achievements of the natural gas industry in China,analyzes the status and challenges of natural gas in the green and low-carbon energy transition,and puts forward the natural gas industry development strategies under carbon neutral target in China.The natural gas industry in China has experienced three periods:start,growth,and leap forward.At present,China has become the fourth largest natural gas producer and third largest natural gas consumer in the world,and has made great achievements in natural gas exploration and development theory and technology,providing important support for the growth of production and reserves.China has set its goal of carbon neutrality to promote green and sustainable development,which brings opportunities and challenges for natural gas industry.Natural gas has significant low-carbon advantages,and gas-electric peak shaving boosts new energy development;the difficulty and cost of development are more prominent.For the national energy security and harmonious development between economy and ecology under the carbon neutral goal,based on the principle of"comprehensive planning,technological innovation,multi-energy complementarity,diversified integration,flexibility and efficiency,optimization and upgrading",the construction of the production-supplystorage-marketing system has to be improved so as to boost the development of the natural gas industry.First,it is necessary to strengthen efforts in the exploration and development of natural gas,making projects and arrangement in key exploration and development areas,meanwhile,it is urgent to make breakthroughs in key science theories and technologies,so as to increase reserve and production.Second,it should promote green and innovative development of the natural gas by developing new techniques,expanding new fields and integrating with new energy.Third,there is a demand to realize transformation and upgrading of the supply and demand structure of natural gas by strengthening the layout of pipeline gas,liquefied natural gas and the construction of underground gas storage,establishing reserve system for improving abilities of emergency response and adjustment,raising the proportion of natural gas in the primary energy consumption and contributing to the transformation of energy consumption structure,realizing low-carbon resources utilization and clean energy consumption.
文摘Investigating the formation mechanisms of carbonate geothermal reservoirs is of theoretical and practical significance for summarizing the formation pattern of geothermal resources and further guiding their effective exploitation.The Beijing-Tianjin-Hebei Plain(BTHP),predominantly located within the Jizhong Depression and Cangxian Uplift in the Bohai Bay Basin,serves as the primary region for geothermal exploitation and utilization in China.More than 1500 geothermal wells have been drilled therein,with water temperature at the wellhead ranging from 55 to 110°C,single-well flow rate ranging between 80 and 120 m^(3)/h,and cumulative heating area exceeding 100×10^(6)m^(3).However,the exploration and research in the region remain limited overall.As per the previous geothermal and petroleum exploration results and the latest geothermal drilling data,this study comprehensively evaluated the geothermal resources of karst geothermal reservoirs.The results show that two suites of carbonate karst reservoirs,namely the Jxw Formation and the Ordovician strata,have primarily developed in the BTHP,and their formation and evolution can be divided into four stages:the Mesoproterozoic-Early Paleozoic stage with carbonate sedimentation and the development of interlayer karst,the Late Paleozoic stage with the development of direct sedimentary cover,the Mesozoic stage with compressional uplifting and development of buried hill karst,and the Cenozoic stage with regional cover deposition and the modification and finalization of karst geothermal reservoirs.Accordingly,the porosity evolution history of the geothermal reservoirs is composed of three stages,namely a significant decrease followed by a minor increase,a gradual decline,and then a small fluctuation from increase to decrease before slowly rising again.The karstification in geothermal reservoirs can be summarized into quasi-syngenetic karstification,epigenetic karstification,and burial karstification,which can be subdivided into seven subcategories.The carbonate geothermal reservoirs in the study area boast total geothermal resources of 53.821×10^(9)GJ,or 184.155×10^(9)t of standard coal equivalent(tce),and the annual exploitable geothermal resources in the urban area can heat an area of(400‒500)×10^(6)m^(3),indicating great potential of geothermal exploitation.
基金supported in part by the Institute for Advanced Study of Central South University and the High Performance Computing Center of Central South Universitythe funding from Guangdong Natural Science Funds(No.2023A0505050107)。
文摘Regulating the catalyst electronic structure is critical for improving the adsorption and catalytic conversion of lithium polysulfides(LiPSs)in lithium-sulfur batteries(Li-S),yet which has been overlooked in current studies.In this work,structurally defined Ag_(30)Pd_(4)nanoclusters were loaded onto reduced graphene oxide(Ag_(30)Pd_(4)/rGO)as a modification material for polypropylene(PP)separators to elucidate the catalytic activity towards lithium polysulfides and the impact on the electrochemical properties to lithium sulfur batteries.This unique d-πcombination promotes charge transfer,influences overall charge states,and further enhances adsorption energies in potential reaction pathways with lithium polysulfides.Consequently,the Ag_(30)Pd_(4)/rGO/PP modified batteries exhibited an exceptionally low-capacity decay rate of 0.026%per cycle at 1.0C over 1000 stable cycles and 9.75 mAh cm^(-2)excellent performance even with lean electrolyte and high sulfur loading(9.7 mg cm^(-2)).This study paves a path for employing ultrasmall bimetallic nanoclusters to promote the polysulfides redox kinetics hence boosting the lithiumsulfur battery performance.
基金supported by the National Natural Science Foundation of China(U2032151,22272059)。
文摘The activity and selectivity of electrocatalytic CO_(2)reduction reaction(CO_(2)RR)to C_(2)products on metal catalysts can be regulated by molecular surfactants.However,the mechanism behind it remains elusive and debatable.Herein,copper nanowires(Cu NWs)were fabricated and decorated with cobalt phthalocyanine(CoPc).The electronic interaction between the Cu NWs,CoPc,CO_(2) and CO_(2)RR intermediates were explored by density functional theory(DFT)calculations.It was found that the selectivity and activity of CO_(2)RR towards C_(2)products on Cu NWs were considerably enhanced from 35.2%to 69.9%by surface decoration of CoPc.DFT calculations revealed that CO_(2)RR can proceed in the interphase between Cu substrate and CoPc,and the CO_(2)RR intermediates could synergistically bond with both Cu and Co metal centre in CuNWs-CoPc,which favours the adsorption of CO_(2),CO and CO_(2)RR intermediates,thus reducing the free energy for CO-COcoupling towards C_(2)products.The synergistic interaction was further extended to phthalocyanine(Pc)and other metal phthalocyanine derivatives(MPc),where a relatively weaker synergistic interaction of COintermediates with MPc and Cu substrate and only a slight enhancement of CO_(2)RR towards C_(2) products were observed.This study demonstrates a synergistic catalysis pathway for CO_(2)RR,a novel perspective in interpreting the role of CoPc in enhancing the activity and selectivity of CO_(2)RR on Cu NWs,in contrast to the conventional tandem catalysis mechanism.
基金the financial support by the National Natural Science Foundation of China(NSFC,grant nos.21905288 and 51904288)Zhejiang Provincial Natural Science Foundation(LZ21B030001)+3 种基金K.C.Wong Education Foundation(GJTD-2019-13)Ningbo major special projects of the Plan“Science and Technology Innovation 2025”(grant nos.2018B10056 and 2019B10046)Ningbo 3315 ProgramYongjiang Talent Introduction Program(no.2021A-115-G)
文摘Developing stable and efficient nonprecious-metal-based oxygen evolution catalysts in the neutral electrolyte is a challenging but essential goal for various electrochemical systems.Particularly,cobalt-based spinels have drawn a considerable amount of attention but most of them operate in alkali solutions.However,the frequently studied Co-Fe spinel system never exhibits appreciable stability in nonbasic conditions,not to mention attract further investigation on its key structural motif and transition states for activity loss.Herein,we report exceptional stable Co-Fe spinel oxygen evolution catalysts(~30%Fe is optimal)in a neutral electrolyte,owing to its unique metal ion arrangements in the crystal lattice.The introduced iron content enters both the octahedral and tetrahedral sites of the spinel as Fe^(2+)and Fe^(3+)(with Co ions having mixed distribution as well).Combining density functional theory calculations,we find that the introduction of Fe to Co_(3)O_(4)lowers the covalency of metal-oxygen bonds and can help suppress the oxidation of Co^(2+/3+)and 0^(2-).It implies that the Co-Fe spinel will have minor surface reconstruction and less lattice oxygen loss during the oxygen evolution reaction process in comparison with Co_(3)O_(4)and hence show much better stability.These findings suggest that there is still much chance for the spinel structures,especially using reasonable sublattices engineering via multimetal doping to develop advanced oxygen evolution catalysts.
基金supported by the National Natural Science Foundation of China (U2032151)the National Key R&D Program of China (2018YFB1502600)+1 种基金the Basic Research and Applied Basic Research Foundation of Guangzhou (B3210580)the Natural Science Foundation of Guangdong Province (B6211050)。
文摘The alkaline hydrogen evolution reaction(HER) on Pt-based catalysts is largely limited by the slow water dissociation kinetics. Pt-based single atom alloy catalysts(SAAC) with water dissociation sites have been demonstrated as excellent alkaline HER catalysts. However, the regulation of their activity and stability at the atomic scale is still a great challenge. Herein, the kinetic and stability issues are successfully resolved via engineering the electronic structure of Pt-Co SAAC by Au-induced tensile strain. The atomic dispersion of Co into the Pt shell was confirmed by extended X-ray absorption fine structure and the electronic structure and catalytic HER performance was modulated by the tensile strain induced by the Pt shell thickness. An inverse volcano-type relation between HER activity and surface strain was found.Density functional theory(DFT) calculations reveal that the Au-induced tensile strain on Pt-Co shell can not only boost the adsorption and dissociation kinetics of water at Co site by upshifting the dband and promoting the electron transfer, but also downshift the d-band center of Pt in Pt-Co shell, leading to optimized H* adsorption/desorption. The champion catalyst provides an overpotential of only 14 m V at the current density of 10 mA cm^(-2). This work not only provides an effective strategy for the construction of single-atom alloy electrocatalysts for high performance toward alkaline HER but also sheds light on the understanding of the reaction mechanism at the atomic level.
基金supported by National Natural Science Foundation of China(No.51276100)the National Basic Research Program of China(973 Program)(No.2013CB228501)the financial funding from the U.S.Department of Energy,Office of Basic Energy Sciences,Chemical Science Division at Lawrence Berkeley National Laboratory(No.2013CB228501)
文摘The carbon content of bituminous coal samples was analyzed by laser-induced breakdown spectroscopy. The 266 nm laser radiation was utilized for laser ablation and plasma generation in air. The partial least square method and the dominant factor bused PLS method were used to improve the measurement accuracy of the carbon content of coal. The results showed that the PLS model could achieve good measurement accuracy, and the dominant factor based PLS model could further improve the measurement accuracy. The coefficient of determination and the root-mean-square error of prediction of the PLS model were 0.97 and 2.19%, respectively; and those values for the dominant factor based PLS model were 0.99 and 1.51%, respectively. The results demonstrated that the 266 nm wavelength could accurately measure the carbon content of bituminous coal.
基金supported by the Fundamental Research Funds for Central Universities(SCUT No.2019ZD22)Guangdong Innovative and Entrepreneurial Research Team Program(No.2016ZT06N569)。
文摘The slow redox dynamics and dissolution of polysulfides in lithium-sulfur(Li-S)batteries result in poor rate performance and rapid decay of battery capacity,thus limiting their practical application.Ferroelectric barium titanate(BT)nanoparticles have been reported to effectively improve the electrochemical performance of Li-S batteries due to the inherent self-polarization and high adsorption capacity of the BT nanoparticles towards polysulfides.Here in this paper,BT nanoparticles,behave as highly efficient electrocatalyst and demonstrate much higher redox dynamics towards the conversion reaction of polysulfides and Li2S than TiO2,as shown by both electrochemical measurements and density functional theory calculation.The coupling of the sulfur host of the hollow and graphitic carbon flakes(HGCF)and the BT nanoparticles(HGCF/S-BT)enable excellent electrochemical performance of Li-S batteries,delivering a0.047%capacity decay per cycle in 1000 cycles at 1 C,788 mAh g^-1 at 2 C and a reversible capacity of613 mAh g^-1 after 300 cycles at a current density of 0.5 C at a S loading of 3.4 mg cm^-2.HGCF/S-BT also shows great promise for practical application in flexible devices as demonstrated on the soft-packaged Li-S batteries.
基金supported by the key R&D program of China Energy Investment Corporation (GJNY-18-27)National Natural Science Foundation of China (Nos. 61675110 and 51906124)。
文摘Laser-induced breakdown spectroscopy(LIBS) is a potential technology for online coal property analysis,but successful quantitative measurement of calorific value using LIBS suffers from relatively low accuracy caused by the matrix effect.To solve this problem,the support vector machine(SVM) and the partial least square(PLS) were combined to increase the measurement accuracy of calorific value in this study.The combination model utilized SVM to classify coal samples into two groups according to their volatile matter contents to reduce the matrix effect,and then applied PLS to establish calibration models for each sample group respectively.The proposed model was applied to the measurement of calorific values of 53 coal samples,showing that the proposed model could greatly increase accuracy of the measurement of calorific values.Compared with the traditional PLS method,the coefficient of determination(R2) was improved from 0.93 to 0.97,the root-mean-square error of prediction was reduced from 1.68 MJ kg-1 to1.08 MJ kg-1,and the average relative error was decreased from 6.7% to 3.93%,showing an overall improvement.
基金the National Key R&D Program of China(2017YFB0603305).
文摘1.Introduction Climate change is one of the most severe challenges facing the world today.At present,China produces total annual carbon dioxide(CO_(2))emissions of over 10 billion tonnes,topping the world in this regard.Although coal empowers China’s economic development,its use presents a great challenge to the nation’s desired goals of peaking carbon emissions and achieving carbon neutrality.In this context,the low-carbon utilization of coal is an inevitable trend for future development.Exploring new ways to reduce CO_(2) emissions on a large scale in the utilization of coal—especially during coal-fired power generation—is essential in order for China to achieve carbon neutrality.
基金Supported by the National Natural Science Foundation of China(42072187)PetroChina Science and Technology Major Project(2021ZZ01-05,2021DJ18).
文摘Carbon dioxide storage and utilization has become an inevitable trend and choice for sustainable development under the background of global climate change and carbon neutrality.Carbon industry which is dominated by CO_(2) capture,utilization and storage/CO_(2) capture and storage(CCUS/CCS)is becoming a new strategic industry under the goal of carbon neutrality.The sustainable development of carbon industry needs to learn from the experiences of global oil and gas industry development.There are three types of“carbon”in the earth system.Black carbon is the CO_(2) that has not been sequestered or used and remains in the atmosphere for a long time;grey carbon is the CO_(2) that has been fixed or permanently sequestered in the geological body,and blue carbon is the CO_(2) that could be converted into products for human use through biological,physical,chemical and other ways.The carbon industry system covers carbon generation,carbon capture,carbon transportation,carbon utilization,carbon sequestration,carbon products,carbon finance,and other businesses.It is a revolutionary industrial field to completely eliminate“black carbon”.The development of carbon industry technical system takes carbon emission reduction,zero carbon,negative carbon and carbon economy as the connotation,and the construction of a low-cost and energy-efficient carbon industry system based on CCUS/CCS are strategic measures to achieve the goal of carbon neutrality and clean energy utilization globally.This will promote the“four 80%s”transformation of China's energy supply,namely,to 2060,the percentage of zero-carbon new energy in the energy consumption will be over 80%and the CO_(2) emission will be decreased by 80%to ensure the carbon emission reduction of total 80×10^(8) t from the percentage of carbon-based fossil energy in the energy consumption of over 80%,and the percentage of CO_(2) emission from energy of over 80%in 2021.The carbon industry in China is facing three challenges,large CO_(2) emissions,high percentage of coal in energy consumption,and poor innovative system.Three strategic measures are proposed accordingly,including:(1)unswervingly develop carbon industrial system and ensure the achievement of carbon neutrality as scheduled by 2060;(2)vigorously develop new energy sources and promote a revolutionary transformation of China’s energy production and consumption structure;(3)accelerate the establishment of scientific and technological innovation system of the whole CO_(2) industry.It is of great significance for continuously optimization of ecological environment and construction of green earth and ecological earth to develop the carbon industry system,utilize clean energy,and achieve the strategic goal of global carbon neutrality.
文摘Nickel-rich layered oxides have been identified as the most promising commercial cathode materials for lithium-ion batteries(LIBs)for their high theoretical specific capacity.However,the poor cycling stability of nickel-rich cathode materials is one of the major barriers for the large-scale usage of LIBs.The existing obstructions that suppress the capacity degradation of nickel-rich cathode materials are as a result of phase transition,mechanical instability,intergranular cracks,side reaction,oxygen loss,and thermal instability during cycling.Core–shell structures,oxidating precursors,electrolyte additives,doping/coating and synthesizing single crystals have been identified as effective methods to improve cycling stability of nickel-rich cathode materials.Herein,recent progress of surface modification,e.g.coating and doping,in nickel-rich cathode materials are summarized based on Periodic table to provide a clear understanding.Electrochemical performances and mechanisms of modified structure are discussed in detail.It is hoped that an overview of synthesis and surface modification can be presented and a perspective of nickel-rich materials in LIBs can be given.
基金supported by the National Key Research and Development Program of China(Grant No.2017YFA0206703)the National Natural Science Foundation of China(Grant No.U2032151)。
文摘The electrochemical performance of lithium-sulfur(Li-S)batteries is strongly hampered by the shuttle effect and slow redox kinetics of lithium polysulfides(Li PSs).Surface modified interlayer of a separator of Li-S batteries is demonstrated to be an effective strategy to overcome this problem.Herein,cobalt nanoparticles confined in nitrogen co-doped porous carbon framework(Co-CN)were developed from pyrolysis of ZIF-67 and used as interlayer of PP separator for Li-S batteries,and were functionalized by four pyrrole derivatives,1-phenylpyrrole,1-methyl pyrrole,1-(p-toluenesulfonyl)pyrrole,and 1-pyrrole,respectively,which were screened in terms of the electron-withdrawing/donating ability of the substituent groups on the pyrrolic nitrogen.The impact of the molecular structure of pyrrole derivatives on the interaction with Li PSs and the electrochemical performance of Li-S batteries were explored by nuclear magnetic resonance and theoretical calculation.It is uncovered that 1-phenylpyrrole shows the highest enhancement of redox kinetics of Li PSs,attributing to the optimal interaction with Co nanoparticles and Li PSs.Therefore,1-phenylpyrrole modified Co-CN interlayer enables the best electrochemical performance for the Li-S batteries,delivering a specific capacity of 562 m Ah g^(-1)at 5 C and a capacity of 538,526,and 449 m Ah g^(-1)after 500 cycles at 1,2,and 3 C,respectively.At a high sulfur loading of 5.5 mg cm^(-2),it achieves a capacity of 440 m Ah g^(-1)after 500 cycles at 1 C.This work reveals the interaction mechanism among Li PSs,Co nanoparticles and the molecular modifiers in improving the electrochemical performance of Li-S batteries.