Zeolites are a promising support for Pd catalysts in leanmethane(CH_(4))combustion.Herein,three types of zeolites(H-MOR,H-ZSM-5 and H-Y)were selected to estimate their structural effects and deactivation mechanisms in...Zeolites are a promising support for Pd catalysts in leanmethane(CH_(4))combustion.Herein,three types of zeolites(H-MOR,H-ZSM-5 and H-Y)were selected to estimate their structural effects and deactivation mechanisms in CH_(4)combustion.We show that variations in zeolite structure and surface acidity led to distinct changes in Pd states.Pd/H-MOR with external high-dispersing Pd nanoparticles exhibited the best apparent activity,with activation energy(Ea)at 73 kJ/mol,while Pd/H-ZSM-5 displayed the highest turnover frequency(TOF)at 19.6×10^(−3)sec^(−1),presumably owing to its large particles with more step sites providing active sites in one particle for CH_(4)activation.Pd/H-Y with dispersed PdO within pore channels and/or Pd2+ions on ion-exchange sites yielded the lowest apparent activity and TOF.Furthermore,Pd/H-MOR and Pd/H-ZSM-5 were both stable under a dry condition,but introducing 3 vol.%H_(2)O caused the CH_(4)conversion rate on Pd/H-MOR drop from 100%to 63%and that on Pd/H-ZSM-5 decreased remarkably from 82%to 36%.The former was shown to originate fromzeolite structural dealumination,and the latter principally owed to Pd aggregation and the loss of active PdO.展开更多
Dehydrogenation of propane(PDH)technology is one of the most promising on-purpose technologies to solve supply-demand unbalance of propylene.The industrial catalysts for PDH,such as Pt-and Cr-based catalysts,still hav...Dehydrogenation of propane(PDH)technology is one of the most promising on-purpose technologies to solve supply-demand unbalance of propylene.The industrial catalysts for PDH,such as Pt-and Cr-based catalysts,still have their own limitation in expensive price and security issues.Thus,a deep understanding into the structure-performance relationship of the catalysts during PDH reaction is necessary to achieve innovation in advanced high-efficient catalysts.In this review,we focused on discussion of structure-performance relationship of catalysts in PDH.Based on analysis of reaction mechanism and nature of active sites,we detailed interaction mechanism between structure of active sites and catalytic performance in metal catalysts and oxide catalysts.The relationship between coke deposition,co-feeding gas,catalytic activity and nanostructure of the catalysts are also highlighted.With these discussions on the relationship between structure and performances,we try to provide the insights into microstructure of active sites in PDH and the rational guidance for future design and development of PDH catalysts.展开更多
Over the past decades,the energy and concomitant environment issues,such as energy shortage,air pollution and global warming,have been becoming increasingly striking world-wide challenges[1,2].Such a dilemma in turn a...Over the past decades,the energy and concomitant environment issues,such as energy shortage,air pollution and global warming,have been becoming increasingly striking world-wide challenges[1,2].Such a dilemma in turn appeals to the development and employment of clean and renewable energy.展开更多
A series of Co/SiO2 catalysts with different sodium （Na）loadings （0, 0.1, 0.2, 0.5 and I wt%） were prepared and evaluated for Fischer-Tropsch reaction to study the effect of Na on the catalyst structure and cataly...A series of Co/SiO2 catalysts with different sodium （Na）loadings （0, 0.1, 0.2, 0.5 and I wt%） were prepared and evaluated for Fischer-Tropsch reaction to study the effect of Na on the catalyst structure and catalytic performance. The addition of Na was found to decrease the catalytic activity and hydrocarbon selectivity, but increase CO2 selec- tivity due to the enhanced WGS activity. The addition of Na also resulted in higher selectivity to oxygenates （alco- hols and aldehydes） and O/P ratio as well as the shift of hydrocarbons to lower carbon numbers. Structure charac- terization revealed a decrease in the surface area and particles size for the calcined samples with the addition of Na. CozC was formed during the reaction process for the Na-promoted catalysts. As a result, a new Co/Co2C bifunc- tional active sites were generated for oxygenates formation leading to increasing oxygenates selectivity. In addition, the Co2C nanoparticles alone may also act as dual active sites for oxygenate formation at high reaction pressure over the promoted catalysts with high Na loading.展开更多
Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.Ho...Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.However,understanding the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance from a comprehensive perspective is crucial for guiding their future development.This review provides a timely and comprehensive overview of the applications of 2D nanomaterials in oil-based lubrication.First,the bottlenecks and mechanisms of action of 2D nanomaterials are outlined,including adsorption protective films,charge adsorption effects,tribochemical reaction films,interlayer slip,and synergistic effects.On this basis,the review summarizes recent structural regulation strategies for 2D nanomaterials,including doping engineering,surface modification,structural optimization,and interfacial mixing engineering.Then,the focus was on analyzing the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance.The effects of thickness,number of layers,sheet diameter,interlayer spacing,Moiré patterns,wettability,functional groups,concentration,as well as interfacial compatibility and dispersion behavior of 2D nanomaterials were systematically investigated in oil-based lubrication,with the intrinsic correlations resolved through computational simulations.Finally,the review offers a preliminary summary of the significant challenges and future directions for 2D nanomaterials in oil-based lubrication.This review aims to provide valuable insights and development strategies for the rational design of high-performance oil-based lubrication materials.展开更多
A thorough understanding of the oxygen evolution reaction(OER)in Mo-based materials is crucial for the advancement of water-splitting technologies.However,the identification of the active phase in Mo-based systems rem...A thorough understanding of the oxygen evolution reaction(OER)in Mo-based materials is crucial for the advancement of water-splitting technologies.However,the identification of the active phase in Mo-based systems remains a subject of debate,largely due to the dissolution of molybdenum oxides in alkaline electrolytes.In this review,we provide a comprehensive overview of recent advances in the application of Mo-based materials for OER in alkaline media,with an emphasis on their diverse roles in catalysis.Various design strategies employed to optimize Mo-based materials are discussed,focusing on how these approaches influence their physicochemical properties and the specific effects of different design perspectives on their OER performance.Additionally,the structure-performance relationship underlying these materials is explored,offering insights into how structural modifications impact catalytic efficiency.Lastly,key challenges for Mo-based materials in OER applications are provided,and future research directions for further improving the efficacy of sustainable water-splitting technologies in alkaline environments are proposed.展开更多
Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalit...Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.展开更多
The relationship mechanism between the material pore structures and cathodic iodine chemistry plays a vital role in efficient Zn-I_(2) batteries,but is unclear,retarding further advances.This work innovatively indicat...The relationship mechanism between the material pore structures and cathodic iodine chemistry plays a vital role in efficient Zn-I_(2) batteries,but is unclear,retarding further advances.This work innovatively indicates a great contribution of∼2.5nm pore structure of nanocarbons to efficient iodine adsorption,rapid I^(−)↔I_(2) conversion,and polyiodide inhibition,via scrupulously designing catalysts with controllable pore sizes systematically.The I_(2)-loading within the designed nitrogen-doped nanocarbons can reach up to as high as 60.8 wt%.The batteries based on the cathode deliver impressive performances with a large capacity of 178.8 mAh/g and long-term cycling stability more than 4000 h at 5.0 C.Notably,these is no polyiodide such as I_(3)−and I_(5)−detected during the charge-discharge processes from comprehensive electrochemical cyclic voltammetry,X-ray photoelectron spectroscopy,and Raman technique.This work provides a novel knowledge-guided concept for rational pore design,promising better Zn-I_(2) batteries,which is also hoped to benefit other advanced energy technologies,such as Li-S,Li-ion,and Al-I_(2) batteries.展开更多
Sodium-ion batteries(SIBs)have been considered as an ideal choice for the next generation large-scale energy storage applications owing to the rich sodium resources and the analogous working principle to that of lithi...Sodium-ion batteries(SIBs)have been considered as an ideal choice for the next generation large-scale energy storage applications owing to the rich sodium resources and the analogous working principle to that of lithium-ion batteries(LIBs).Nevertheless,the larger size and heavier mass of Na^(+)ion than those of Li^(+)ion often lead to sluggish reaction kinetics and inferior cycling life in SIBs compared to the LIB counterparts.The pursuit of promising electrode materials that can accommodate the rapid and stable Na-ion insertion/extraction is the key to promoting the development of SIBs toward a commercial prosperity.One-dimensional(1 D)nanomaterials demonstrate great prospects in boosting the rate and cycling performances because of their large active surface areas,high endurance for deformation stress,short ions diffusion channels,and oriented electrons transfer paths.Electrospinning,as a versatile synthetic technology,features the advantages of controllable preparation,easy operation,and mass production,has been widely applied to fabricate the 1 D nanostructured electrode materials for SIBs.In this review,we comprehensively summarize the recent advances in the sodium-storage cathode and anode materials prepared by electrospinning,discuss the effects of modulating the spinning parameters on the materials’micro/nano-structures,and elucidate the structure-performance correlations of the tailored electrodes.Finally,the future directions to harvest more breakthroughs in electrospun Na-storage materials are pointed out.展开更多
Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of ...Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of CO_(2) and the storage of renewable energy are realized.The reactivity and selectivity of CO_(2)RR depend on the structure and composition of the catalyst,applied potential,electrolyte,and pH of the solution.Besides,multiple electron and proton transfer steps are involved in CO_(2)RR,making the reaction pathways even more complicated.In pursuit of molecular-level insights into the CO_(2)RR processes,in situ vibrational methods including infrared,Raman and sum frequency generation spectroscopies have been deployed to monitor the dynamic evolution of catalyst structure,to identify reactive intermediates as well as to investigate the effect of local reaction environment on CO_(2)RR performance.This review summarizes key findings from recent electrochemical vibrational spectrosopic studies of CO_(2)RR in addressing the following issues:the CO_(2)RR mechanisms of different pathways,the role of surface-bound CO species,the compositional and structural effects of catalysts and electrolytes on CO_(2)RR activity and selectivity.Our perspectives on developing high sensitivity wide-frequency infrared spectroscopy,coupling different spectroelectrochemical methods and implementing operando vibrational spectroscopies to tackle the CO_(2)RR process in pilot reactors are offered at the end.展开更多
Energy storage is an ever-growing global concern due to increased energy needs and resource exhaustion.Sodium-ion batteries(SIBs)have called increasing attention and achieved substantial progress in recent years owing...Energy storage is an ever-growing global concern due to increased energy needs and resource exhaustion.Sodium-ion batteries(SIBs)have called increasing attention and achieved substantial progress in recent years owing to the abundance and even distribution of Na resources in the crust,and the predicted low cost of the technique.Nevertheless,SIBs still face challenges like lower energy density and inferior cycling stability compared to mature lithium-ion batteries(LIBs).Enhancing the electrochemical performance of SIBs requires an in-deep and comprehensive understanding of the improvement strategies and the underlying reaction mechanism elucidated by in situ techniques.In this review,commonly applied in situ techniques,for instance,transmission electron microscopy(TEM),Raman spectroscopy,X-ray diffraction(XRD),and X-ray absorption near-edge structure(XANES),and their applications on the representative cathode and anode materials with selected samples are summarized.We discuss the merits and demerits of each type of material,strategies to enhance their electrochemical performance,and the applications of in situ characterizations of them during the de/sodiation process to reveal the underlying reaction mechanism for performance improvement.We aim to elucidate the composition/structure-per formance relationship to provide guidelines for rational design and preparation of electrode materials toward high electrochemical performance.展开更多
A highly efficient and green process was developed for the synthesis of useful 5-amino-1-pentanol(5-AP)from biomass-derived dihydropyran by coupling the in situ generation of 5-hydroxypentanal(5-HP,via the ring-openin...A highly efficient and green process was developed for the synthesis of useful 5-amino-1-pentanol(5-AP)from biomass-derived dihydropyran by coupling the in situ generation of 5-hydroxypentanal(5-HP,via the ring-opening tautomerization of 2-hydroxytetrahydropyran(2-HTHP))and its reductive amination over supported Ni catalysts.The catalytic performances of the supported Ni catalysts on different oxides including SiO2,TiO2,ZrO2,γ-Al2 O3,and MgO as well as several commercial hydrogenation catalysts were investigated.The Ni/ZrO2 catalyst presented the highest 5-AP yield.The characterization results of the oxide-supported Ni catalysts showed that the Ni/ZrO2 catalyst possessed high reducibility and a high surface acid density,which lead to the enhanced activity and selectivity of the catalyst.The effect of reaction parameters on the catalytic performance of the Ni/ZrO2 catalyst was studied,and a high 5-AP yield of 90.8%was achieved in the reductive amination of 2-HTHP aqueous solution under mild conditions of 80℃and 2 MPa H2.The stability of the Ni/ZrO2 catalyst was studied using a continuous flow reactor,and only a slight decrease in the 5-AP yield was observed after a 90-h time-on-stream.Additionally,the reaction pathways for the reductive amination of 2-HTHP to synthesize 5-AP were proposed.展开更多
Supported nickel catalysts are promising candidates for dry reforming of methane, but agglomeration of Ni^(0) and coke deposition hinder the industrial applications. Herein, we report a novel interface-directed synthe...Supported nickel catalysts are promising candidates for dry reforming of methane, but agglomeration of Ni^(0) and coke deposition hinder the industrial applications. Herein, we report a novel interface-directed synthetic approach to construct distinct metal ensembles by carefully tuning the compositions of the carriers. A Zr-Mn-Zn ternary oxide-supported Ni catalyst, together with the respective binary oxide-supported analogues, was synthesized by adopting a sequential co-precipitation and wetness impregnation method. Combined characterization techniques identify distinct catalyst models, including (i) conventional NiO nanoparticles with different sizes on Zr-Mn and Zr-Zn, and (ii) epitaxially growing NiO ensembles of a few nanometers thickness at the periphery of ZnO_(x) particles. These catalysts exhibit divergent responses in the catalytic testing, with the ternary oxide system significantly outperforming the binary analogues. The strong electronic interactions between Mn-Ni increase Ni dispersion and the activity while the stability is strengthened upon Zn addition. Both high activity, high selectivity, and remarkable stability are attained upon co-adding Mn and Zn. The interfaces between Ni and Zr-Mn-Zn rather than the physical contacts of individual oxide-supported analogues through mechanical mixing are keys for the outstanding performance.展开更多
Complex coordinated functional groups[MA_(x)B_(y)](M=Central coordination element;A,B=P,O,S,Se,F,Cl,Br or I)are composed of different types of anions A,B jointly linked to the same central cation M,which are in high p...Complex coordinated functional groups[MA_(x)B_(y)](M=Central coordination element;A,B=P,O,S,Se,F,Cl,Br or I)are composed of different types of anions A,B jointly linked to the same central cation M,which are in high potential to tune the physical properties of materials,e.g.,second-order susceptibility,energy gaps and birefringence.Recently,Compound containing complex coordinated functional groups have attracted great attention in the nonlinear optical(NLO)field and a large number of this type crystals exhibit promising NLO performance.However,the inherent relationship between ionic group structure and optical properties of complex coordinated NLO materials have not been systematically studied.This article systematically summarizes complex coordinated NLO materials in recent five years from the perspective of the internal relationship between crystal structure and optical properties.In addition,we propose the ideal combination and arrangement modes for structural building units,and also reveal the influence of complex coordinated functional groups[MA_(x)B_(y)]toward the NLO response,optical band gap and phase matching ability of complex coordinated NLO materials.展开更多
Since the 1980s,single-crystal Pt electrodes with well-defined surface structures have been deemed stable under mild electrochemical conditions(e.g.,in the potential region of electric double layers,underpotential dep...Since the 1980s,single-crystal Pt electrodes with well-defined surface structures have been deemed stable under mild electrochemical conditions(e.g.,in the potential region of electric double layers,underpotential deposition of hydrogen,or mild hydrogen evolution/OH adsorption)and have served as model electrodes for unraveling the structure-performance relation in electrocatalysis.With the advancement of in situ electrochemical microscopy/spectroscopy techniques,subtle surface restructuring under mild electrochemical conditions has been achieved in the last decade.Surface restructuring can considerably modify electrocatalytic properties by generating/destroying highly active sites,thereby interfering with the deduction of the structure-performance relation.In this review,we summarize recent progress in the restructuring of well-defined Pt(-based)electrode surfaces under mild electrochemical conditions.The importance of the meticulous structural characterization of Pt electrodes before,during,and after electrochemical measurements is demonstrated using CO adsorption/oxidation,hydrogen adsorption/evolution,and oxygen reduction as examples.The implications of present findings for correctly identifying the reaction mechanisms and kinetics of other electrocatalytic systems are also briefly discussed.展开更多
Supercapacitors formed from porous carbon and graphene-oxide(GO)materials are usually dominated by either electric double-layer capacitance,pseudo-capacitance,or both.Due to these combined features,reduced GO material...Supercapacitors formed from porous carbon and graphene-oxide(GO)materials are usually dominated by either electric double-layer capacitance,pseudo-capacitance,or both.Due to these combined features,reduced GO materials have been shown to offer superior capacitance over typical nanoporous carbon materials;however,there is a significant variation in reported values,ranging between 25 and 350 F g^(−1).This undermines the structure(e.g.,oxygen functionality and/or surface area)-performance relationships for optimization of cost and scalable factors.This work demonstrates important structure-controlled charge storage relationships.For this,a series of exfoliated graphene(EG)derivatives are produced via thermal-shock exfoliation of GO precursors and following controlled graphitization of EG(GEG)generates materials with varied amounts of porosity,redox-active oxygen groups and graphitic components.Experimental results show significantly varied capacitance values between 30 and 250 F g^(−1)at 1.0 A g^(−1)in GEG structures;this suggests that for a given specific surface area the redox-active and hydrophilic oxygen content can boost the capacitance to 250–300%higher compared to typical mesoporous carbon materials.GEGs with identical oxygen functionality show a surface area governed capacitance.This allows to establish direct structure-performance relationships between 1)redox-active oxygen functional concentration and capacitance and 2)surface area and capacitance.展开更多
Direct synthesis of H_(2)O_(2)from H_(2) and O_(2)via heterogeneous catalysis is an environmentally friendly and atomically economic alternative to the traditional anthraquinone oxidation(AO)process.Optimizing the ele...Direct synthesis of H_(2)O_(2)from H_(2) and O_(2)via heterogeneous catalysis is an environmentally friendly and atomically economic alternative to the traditional anthraquinone oxidation(AO)process.Optimizing the electronic and geometric structures of the active metals to break the current limitations of hydrogenation rate and H_(2)O_(2)selectivity is a promising and challenging topic.In this study,a series of Pd-Au bimetallic catalysts supported on TiO_(2)with a metal loading of 3.0 wt%and a constant Pd/Au molar ratio(Pd:Au=2:1)were prepared.The catalysts were reduced in H_(2) at different temperatures(473,573 and 673 K),and their catalytic activity for the direct H_(2)O_(2)synthesis were evaluated at 283 K and 0.1MPa.H_(2) reduced Pd-Au catalysts exhibited superior performance in direct H_(2)O_(2)synthesis.The maximum H_(2)O_(2)selectivity of 87.7%and H_(2)O_(2)yield of 3116.4 mmol h^(−1) gPd^(−1) were achieved over the Pd_(2.0)Au_(1.0)-573 catalyst with a H_(2) conversion of 12.8%.The tailored local chemical environment caused by H_(2) reduction creates a balanced ratio of Pd0 and PdO_(x) sites,thus improving the selectivity towards H_(2)O_(2).This work developed an effective strategy for fabrication of highly active and stable Pd-based H_(2)O_(2)synthesis catalysts with high H_(2)O_(2)yield.展开更多
Cu-based nanomaterials have demonstrated great potential for catalyzing the electrosynthesis of oxime compounds,a type of organonitrogen molecule that finds versatile applications in the pharmaceutical industry,medici...Cu-based nanomaterials have demonstrated great potential for catalyzing the electrosynthesis of oxime compounds,a type of organonitrogen molecule that finds versatile applications in the pharmaceutical industry,medicine production,chemical feedstocks,and other fields.This review first explains the significance of oxime compounds and compares the conventional synthetic approach with the emerging electrochemical method.Then,the Cu-based nanomaterials including Cu-based com-pounds/composites,Cu-based bimetallic alloys,Cu-based high entropy alloys,and Cu-based single-atom catalysts for oxime electrosynthesis are described with some explicit examples to elucidate the structure-performance relationship clearly.Finally,the current challenges and future perspectives of this rapidly developing and evolving field are analyzed with some critical thoughts.This review is anticipated to stimulate more research efforts to be dedicated to this fast-growing yet quite promising field.展开更多
Transfer hydrogenation(TH)has become the new frontier of hydrogenation science owing to the use of non-H2 hydrogen sources which are safer and easier handling for constructing various hydrogenated products.As for hete...Transfer hydrogenation(TH)has become the new frontier of hydrogenation science owing to the use of non-H2 hydrogen sources which are safer and easier handling for constructing various hydrogenated products.As for heterogeneous catalysts applied for TH which take advantages of convenient separation and recycling,single-atom catalysts(SACs)are attractive alternatives because of their maximum atom utilization,well-defined active sites and tunable local atomic structure.Recent literature has manifested the good performance of SACs for TH,gaining attention both from academia and industry.In this perspective,we review TH achieved by SACs according to classified hydrogen sources and provide a comprehensive understanding of the relationship between their structural characters and performance for TH.In addition,corresponding synthetic strategies of SACs are also demonstrated to reveal their roles in forming the featured structures.The remained challenges and potential opportunities in this field are also discussed in the end.This review will guide the design of better-performing SACs for TH and give an impetus to the development of green and cost-effective hydrogenation technology.展开更多
Acceptor-donor-acceptor(A-D-A)-type nonfullerene acceptors(NFAs)have contributed to an efficiency breakthrough in organic solar cells(OSCs).However,the absence of an in-depth understanding of how to achieve high charg...Acceptor-donor-acceptor(A-D-A)-type nonfullerene acceptors(NFAs)have contributed to an efficiency breakthrough in organic solar cells(OSCs).However,the absence of an in-depth understanding of how to achieve high charge generation probability while guaranteeing low energy loss by molecular design has caused the stagnation of power conversion efficiency(PCE)in A-D-A-type acceptors.The fluorination strategy,as an effective approach to regulating molecular photoelectric and aggregation properties,can significantly affect device performance in OSCs.However,a comprehensive understanding of the relationship between fluorination and photovoltaic performance has been scarcely investigated thus far.Herein,a series of A-D-A-type acceptors,named ZITI-N-nF(n=2,4,6,8,representing the number of fluorine atoms),were designed and synthesized to reveal the underlying work mechanism of OSCs with low energy loss and efficient charge generation via fine-tuning of the charge-transfer state.The results indicate that ZITI-N-6F-based devices exhibit impressive charge generation probability with low energy loss(Eloss)because of the reduced nonradiative recombination,thus leading to a high PCE of 16.11%in binary OSCs and a PCE of 17.09%in ternary OSCs.Notably,a PCE of 16.6%was verified by the National Institute of Metrology,China,which is the highest certified PCE among OSCs based on A-D-A-type NFAs.展开更多
基金supported by the National Key R&D Program of China(No.2022YFC3701603)the National Natural Science Foundation of China(Nos.22106133,52070168)+1 种基金the Key R&D Plan of Zhejiang Province(No.2023C03127)the Fundamental Research Funds for the Central Universities(No.226-2022-00150).
文摘Zeolites are a promising support for Pd catalysts in leanmethane(CH_(4))combustion.Herein,three types of zeolites(H-MOR,H-ZSM-5 and H-Y)were selected to estimate their structural effects and deactivation mechanisms in CH_(4)combustion.We show that variations in zeolite structure and surface acidity led to distinct changes in Pd states.Pd/H-MOR with external high-dispersing Pd nanoparticles exhibited the best apparent activity,with activation energy(Ea)at 73 kJ/mol,while Pd/H-ZSM-5 displayed the highest turnover frequency(TOF)at 19.6×10^(−3)sec^(−1),presumably owing to its large particles with more step sites providing active sites in one particle for CH_(4)activation.Pd/H-Y with dispersed PdO within pore channels and/or Pd2+ions on ion-exchange sites yielded the lowest apparent activity and TOF.Furthermore,Pd/H-MOR and Pd/H-ZSM-5 were both stable under a dry condition,but introducing 3 vol.%H_(2)O caused the CH_(4)conversion rate on Pd/H-MOR drop from 100%to 63%and that on Pd/H-ZSM-5 decreased remarkably from 82%to 36%.The former was shown to originate fromzeolite structural dealumination,and the latter principally owed to Pd aggregation and the loss of active PdO.
基金supported by the National Natural Science Foundation of China(21872163,21972166)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2017A05)+1 种基金Beijing Natural Science Foundation(2202045,2182060)PetroChina Innovation Foundation(2018D-5007-0505)
文摘Dehydrogenation of propane(PDH)technology is one of the most promising on-purpose technologies to solve supply-demand unbalance of propylene.The industrial catalysts for PDH,such as Pt-and Cr-based catalysts,still have their own limitation in expensive price and security issues.Thus,a deep understanding into the structure-performance relationship of the catalysts during PDH reaction is necessary to achieve innovation in advanced high-efficient catalysts.In this review,we focused on discussion of structure-performance relationship of catalysts in PDH.Based on analysis of reaction mechanism and nature of active sites,we detailed interaction mechanism between structure of active sites and catalytic performance in metal catalysts and oxide catalysts.The relationship between coke deposition,co-feeding gas,catalytic activity and nanostructure of the catalysts are also highlighted.With these discussions on the relationship between structure and performances,we try to provide the insights into microstructure of active sites in PDH and the rational guidance for future design and development of PDH catalysts.
基金supported by the National Natural Science Foundation of China(51972024,51702013,51902025)the Fundamental Research Funds for the Central Universities(FRF-BD-20-07A,2019NTST29)+1 种基金the Scientific and Technological Innovation Foundation of Shunde Graduate School,University of Science and Technology Beijing(BK19AE029)funding from China Scholarship Council。
文摘Over the past decades,the energy and concomitant environment issues,such as energy shortage,air pollution and global warming,have been becoming increasingly striking world-wide challenges[1,2].Such a dilemma in turn appeals to the development and employment of clean and renewable energy.
基金This work has been supported by the National Natu- ral Science Foundation of China （Nos. 91545112, 21573271, 21403278）, Shanghai Municipal Science and Technology Commission, China （No. 15DZ1170500）and the Chinese Academy of Sciences （No. QYZDB- SSW-SLH035, Youth Innovation Promotion Association）.
文摘A series of Co/SiO2 catalysts with different sodium （Na）loadings （0, 0.1, 0.2, 0.5 and I wt%） were prepared and evaluated for Fischer-Tropsch reaction to study the effect of Na on the catalyst structure and catalytic performance. The addition of Na was found to decrease the catalytic activity and hydrocarbon selectivity, but increase CO2 selec- tivity due to the enhanced WGS activity. The addition of Na also resulted in higher selectivity to oxygenates （alco- hols and aldehydes） and O/P ratio as well as the shift of hydrocarbons to lower carbon numbers. Structure charac- terization revealed a decrease in the surface area and particles size for the calcined samples with the addition of Na. CozC was formed during the reaction process for the Na-promoted catalysts. As a result, a new Co/Co2C bifunc- tional active sites were generated for oxygenates formation leading to increasing oxygenates selectivity. In addition, the Co2C nanoparticles alone may also act as dual active sites for oxygenate formation at high reaction pressure over the promoted catalysts with high Na loading.
基金supported by the National Natural Science Foundation of China(No.51874036)the Natural Science Foundation of Ningxia(No.2024AAC02034)。
文摘Two-dimensional(2D) nanomaterials have always been regarded as having great development potential in the field of oil-based lubrication due to their designable structures,functional groups,and abundant active sites.However,understanding the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance from a comprehensive perspective is crucial for guiding their future development.This review provides a timely and comprehensive overview of the applications of 2D nanomaterials in oil-based lubrication.First,the bottlenecks and mechanisms of action of 2D nanomaterials are outlined,including adsorption protective films,charge adsorption effects,tribochemical reaction films,interlayer slip,and synergistic effects.On this basis,the review summarizes recent structural regulation strategies for 2D nanomaterials,including doping engineering,surface modification,structural optimization,and interfacial mixing engineering.Then,the focus was on analyzing the structure-performance relationship between the chemical structure of 2D nanomaterials and their lubrication performance.The effects of thickness,number of layers,sheet diameter,interlayer spacing,Moiré patterns,wettability,functional groups,concentration,as well as interfacial compatibility and dispersion behavior of 2D nanomaterials were systematically investigated in oil-based lubrication,with the intrinsic correlations resolved through computational simulations.Finally,the review offers a preliminary summary of the significant challenges and future directions for 2D nanomaterials in oil-based lubrication.This review aims to provide valuable insights and development strategies for the rational design of high-performance oil-based lubrication materials.
基金financially supported by the National Natural Science Foundation of China(52162036 and 22378342)the Key Project of Nature Science Foundation of Xinjiang(2021D01D08)+1 种基金the Major Projects of Xinjiang(2022A01005-4 and 2021A01001-1)the Key Research and Development Project of Xinjiang(2023B01025-1)。
文摘A thorough understanding of the oxygen evolution reaction(OER)in Mo-based materials is crucial for the advancement of water-splitting technologies.However,the identification of the active phase in Mo-based systems remains a subject of debate,largely due to the dissolution of molybdenum oxides in alkaline electrolytes.In this review,we provide a comprehensive overview of recent advances in the application of Mo-based materials for OER in alkaline media,with an emphasis on their diverse roles in catalysis.Various design strategies employed to optimize Mo-based materials are discussed,focusing on how these approaches influence their physicochemical properties and the specific effects of different design perspectives on their OER performance.Additionally,the structure-performance relationship underlying these materials is explored,offering insights into how structural modifications impact catalytic efficiency.Lastly,key challenges for Mo-based materials in OER applications are provided,and future research directions for further improving the efficacy of sustainable water-splitting technologies in alkaline environments are proposed.
基金supported by the open funds of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, Chinathe funding from Guangdong Natural Science Funds (No. 2023A0505050107)。
文摘Atomically precise metal nanoclusters are an emerging type of nanomaterial which has diverse interfacial metal-ligand coordination motifs that can significantly affect their physicochemical properties and functionalities.Among that,Cu nanoclusters have been gaining continuous increasing research attentions,thanks to the low cost,diversified structures,and superior catalytic performance for various reactions.In this review,we first summarize the recent progress regarding the synthetic methods of atomically precise Cu nanoclusters and the coordination modes between Cu and several typical ligands and then discuss the catalytic applications of these Cu nanoclusters with some explicit examples to explain the atomical-level structure-performance relationship.Finally,the current challenges and future research perspectives with some critical thoughts are elaborated.We hope this review can not only provide a whole picture of the current advances regarding the synthesis and catalytic applications of atomically precise Cu nanoclusters,but also points out some future research visions in this rapidly booming field.
基金supported by the Tianjin Natural Science Foundation of China(Nos.20JCZDJC00280 and 20JCYBJC00380).
文摘The relationship mechanism between the material pore structures and cathodic iodine chemistry plays a vital role in efficient Zn-I_(2) batteries,but is unclear,retarding further advances.This work innovatively indicates a great contribution of∼2.5nm pore structure of nanocarbons to efficient iodine adsorption,rapid I^(−)↔I_(2) conversion,and polyiodide inhibition,via scrupulously designing catalysts with controllable pore sizes systematically.The I_(2)-loading within the designed nitrogen-doped nanocarbons can reach up to as high as 60.8 wt%.The batteries based on the cathode deliver impressive performances with a large capacity of 178.8 mAh/g and long-term cycling stability more than 4000 h at 5.0 C.Notably,these is no polyiodide such as I_(3)−and I_(5)−detected during the charge-discharge processes from comprehensive electrochemical cyclic voltammetry,X-ray photoelectron spectroscopy,and Raman technique.This work provides a novel knowledge-guided concept for rational pore design,promising better Zn-I_(2) batteries,which is also hoped to benefit other advanced energy technologies,such as Li-S,Li-ion,and Al-I_(2) batteries.
基金Financial support from the National Natural Science Foundation of China(21805007)Young Elite Scientists Sponsorship Program by CAST(2018QNRC001)+3 种基金Beijing Natural Science Foundation(L182019)National Key Research and Development Program of China(2018YFB0104300)Fundamental Research Funds for the Central Universities(FRF-TP-19-029A2)111 Project(B12015)。
文摘Sodium-ion batteries(SIBs)have been considered as an ideal choice for the next generation large-scale energy storage applications owing to the rich sodium resources and the analogous working principle to that of lithium-ion batteries(LIBs).Nevertheless,the larger size and heavier mass of Na^(+)ion than those of Li^(+)ion often lead to sluggish reaction kinetics and inferior cycling life in SIBs compared to the LIB counterparts.The pursuit of promising electrode materials that can accommodate the rapid and stable Na-ion insertion/extraction is the key to promoting the development of SIBs toward a commercial prosperity.One-dimensional(1 D)nanomaterials demonstrate great prospects in boosting the rate and cycling performances because of their large active surface areas,high endurance for deformation stress,short ions diffusion channels,and oriented electrons transfer paths.Electrospinning,as a versatile synthetic technology,features the advantages of controllable preparation,easy operation,and mass production,has been widely applied to fabricate the 1 D nanostructured electrode materials for SIBs.In this review,we comprehensively summarize the recent advances in the sodium-storage cathode and anode materials prepared by electrospinning,discuss the effects of modulating the spinning parameters on the materials’micro/nano-structures,and elucidate the structure-performance correlations of the tailored electrodes.Finally,the future directions to harvest more breakthroughs in electrospun Na-storage materials are pointed out.
文摘Using renewable energy to drive carbon dioxide reduction reaction(CO_(2)RR)electrochemically into chemicals with high energy density is an efficient way to achieve carbon neutrality,where the effective utilization of CO_(2) and the storage of renewable energy are realized.The reactivity and selectivity of CO_(2)RR depend on the structure and composition of the catalyst,applied potential,electrolyte,and pH of the solution.Besides,multiple electron and proton transfer steps are involved in CO_(2)RR,making the reaction pathways even more complicated.In pursuit of molecular-level insights into the CO_(2)RR processes,in situ vibrational methods including infrared,Raman and sum frequency generation spectroscopies have been deployed to monitor the dynamic evolution of catalyst structure,to identify reactive intermediates as well as to investigate the effect of local reaction environment on CO_(2)RR performance.This review summarizes key findings from recent electrochemical vibrational spectrosopic studies of CO_(2)RR in addressing the following issues:the CO_(2)RR mechanisms of different pathways,the role of surface-bound CO species,the compositional and structural effects of catalysts and electrolytes on CO_(2)RR activity and selectivity.Our perspectives on developing high sensitivity wide-frequency infrared spectroscopy,coupling different spectroelectrochemical methods and implementing operando vibrational spectroscopies to tackle the CO_(2)RR process in pilot reactors are offered at the end.
基金supported by the National Natural Science Foundation of China(22005130,21925404,21902137,21991151,and 22021001)the National Key Research and Development Program of China(2019YFA0705400 and 2020YFB1505800)the Natural Science Foundation of Fujian Province of China(2021J01988)。
文摘Energy storage is an ever-growing global concern due to increased energy needs and resource exhaustion.Sodium-ion batteries(SIBs)have called increasing attention and achieved substantial progress in recent years owing to the abundance and even distribution of Na resources in the crust,and the predicted low cost of the technique.Nevertheless,SIBs still face challenges like lower energy density and inferior cycling stability compared to mature lithium-ion batteries(LIBs).Enhancing the electrochemical performance of SIBs requires an in-deep and comprehensive understanding of the improvement strategies and the underlying reaction mechanism elucidated by in situ techniques.In this review,commonly applied in situ techniques,for instance,transmission electron microscopy(TEM),Raman spectroscopy,X-ray diffraction(XRD),and X-ray absorption near-edge structure(XANES),and their applications on the representative cathode and anode materials with selected samples are summarized.We discuss the merits and demerits of each type of material,strategies to enhance their electrochemical performance,and the applications of in situ characterizations of them during the de/sodiation process to reveal the underlying reaction mechanism for performance improvement.We aim to elucidate the composition/structure-per formance relationship to provide guidelines for rational design and preparation of electrode materials toward high electrochemical performance.
基金supported by the National Natural Science Foundation of China(21872155,21473224)Cooperation Foundation of Dalian National Laboratory for Clean Energy(DNL 180303)+2 种基金Key Research Project of Frontier Science of Chinese Academy of Sciences(QYZDJ-SSW-SLH051)the Youth Innovation Promotion Association,CAS(2016371)the Suzhou Science and Technology Development Plan(SYG201626)~~
文摘A highly efficient and green process was developed for the synthesis of useful 5-amino-1-pentanol(5-AP)from biomass-derived dihydropyran by coupling the in situ generation of 5-hydroxypentanal(5-HP,via the ring-opening tautomerization of 2-hydroxytetrahydropyran(2-HTHP))and its reductive amination over supported Ni catalysts.The catalytic performances of the supported Ni catalysts on different oxides including SiO2,TiO2,ZrO2,γ-Al2 O3,and MgO as well as several commercial hydrogenation catalysts were investigated.The Ni/ZrO2 catalyst presented the highest 5-AP yield.The characterization results of the oxide-supported Ni catalysts showed that the Ni/ZrO2 catalyst possessed high reducibility and a high surface acid density,which lead to the enhanced activity and selectivity of the catalyst.The effect of reaction parameters on the catalytic performance of the Ni/ZrO2 catalyst was studied,and a high 5-AP yield of 90.8%was achieved in the reductive amination of 2-HTHP aqueous solution under mild conditions of 80℃and 2 MPa H2.The stability of the Ni/ZrO2 catalyst was studied using a continuous flow reactor,and only a slight decrease in the 5-AP yield was observed after a 90-h time-on-stream.Additionally,the reaction pathways for the reductive amination of 2-HTHP to synthesize 5-AP were proposed.
基金financial supports from the Zhejiang Normal University(YS304320035)the Natural Science Foundation of China(21603039)。
文摘Supported nickel catalysts are promising candidates for dry reforming of methane, but agglomeration of Ni^(0) and coke deposition hinder the industrial applications. Herein, we report a novel interface-directed synthetic approach to construct distinct metal ensembles by carefully tuning the compositions of the carriers. A Zr-Mn-Zn ternary oxide-supported Ni catalyst, together with the respective binary oxide-supported analogues, was synthesized by adopting a sequential co-precipitation and wetness impregnation method. Combined characterization techniques identify distinct catalyst models, including (i) conventional NiO nanoparticles with different sizes on Zr-Mn and Zr-Zn, and (ii) epitaxially growing NiO ensembles of a few nanometers thickness at the periphery of ZnO_(x) particles. These catalysts exhibit divergent responses in the catalytic testing, with the ternary oxide system significantly outperforming the binary analogues. The strong electronic interactions between Mn-Ni increase Ni dispersion and the activity while the stability is strengthened upon Zn addition. Both high activity, high selectivity, and remarkable stability are attained upon co-adding Mn and Zn. The interfaces between Ni and Zr-Mn-Zn rather than the physical contacts of individual oxide-supported analogues through mechanical mixing are keys for the outstanding performance.
基金supported by National Natural Science Founda-tion of China(No.51972208).
文摘Complex coordinated functional groups[MA_(x)B_(y)](M=Central coordination element;A,B=P,O,S,Se,F,Cl,Br or I)are composed of different types of anions A,B jointly linked to the same central cation M,which are in high potential to tune the physical properties of materials,e.g.,second-order susceptibility,energy gaps and birefringence.Recently,Compound containing complex coordinated functional groups have attracted great attention in the nonlinear optical(NLO)field and a large number of this type crystals exhibit promising NLO performance.However,the inherent relationship between ionic group structure and optical properties of complex coordinated NLO materials have not been systematically studied.This article systematically summarizes complex coordinated NLO materials in recent five years from the perspective of the internal relationship between crystal structure and optical properties.In addition,we propose the ideal combination and arrangement modes for structural building units,and also reveal the influence of complex coordinated functional groups[MA_(x)B_(y)]toward the NLO response,optical band gap and phase matching ability of complex coordinated NLO materials.
文摘Since the 1980s,single-crystal Pt electrodes with well-defined surface structures have been deemed stable under mild electrochemical conditions(e.g.,in the potential region of electric double layers,underpotential deposition of hydrogen,or mild hydrogen evolution/OH adsorption)and have served as model electrodes for unraveling the structure-performance relation in electrocatalysis.With the advancement of in situ electrochemical microscopy/spectroscopy techniques,subtle surface restructuring under mild electrochemical conditions has been achieved in the last decade.Surface restructuring can considerably modify electrocatalytic properties by generating/destroying highly active sites,thereby interfering with the deduction of the structure-performance relation.In this review,we summarize recent progress in the restructuring of well-defined Pt(-based)electrode surfaces under mild electrochemical conditions.The importance of the meticulous structural characterization of Pt electrodes before,during,and after electrochemical measurements is demonstrated using CO adsorption/oxidation,hydrogen adsorption/evolution,and oxygen reduction as examples.The implications of present findings for correctly identifying the reaction mechanisms and kinetics of other electrocatalytic systems are also briefly discussed.
基金supported by EPSRC(grants of EP/R511638/1,EP/S018204/2,EP/R023581/1,EP/W03395X/1,EP/W033321/1)the Science Specialty Program of Sichuan University(Grant.No.2020SCUNL210)+2 种基金The Royal Academy of Engineering is acknowledged for the financial support of Shearing(Ci ET171859)Brett(RCSRF2021/13/53)under the Research Chairs and Senior Research Fel owships schemethe National Physical Laboratory(NPL)and HORIBA MIRA for the support of his RAEng Research Chair
文摘Supercapacitors formed from porous carbon and graphene-oxide(GO)materials are usually dominated by either electric double-layer capacitance,pseudo-capacitance,or both.Due to these combined features,reduced GO materials have been shown to offer superior capacitance over typical nanoporous carbon materials;however,there is a significant variation in reported values,ranging between 25 and 350 F g^(−1).This undermines the structure(e.g.,oxygen functionality and/or surface area)-performance relationships for optimization of cost and scalable factors.This work demonstrates important structure-controlled charge storage relationships.For this,a series of exfoliated graphene(EG)derivatives are produced via thermal-shock exfoliation of GO precursors and following controlled graphitization of EG(GEG)generates materials with varied amounts of porosity,redox-active oxygen groups and graphitic components.Experimental results show significantly varied capacitance values between 30 and 250 F g^(−1)at 1.0 A g^(−1)in GEG structures;this suggests that for a given specific surface area the redox-active and hydrophilic oxygen content can boost the capacitance to 250–300%higher compared to typical mesoporous carbon materials.GEGs with identical oxygen functionality show a surface area governed capacitance.This allows to establish direct structure-performance relationships between 1)redox-active oxygen functional concentration and capacitance and 2)surface area and capacitance.
基金supported by the National Natural Science Foundation of China(Nos.91934302 and 22178110)the Dean/Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(No.2020K001)the Project of the Department of Science and Technology of Sichuan Province(No.2023YFQ0086).
文摘Direct synthesis of H_(2)O_(2)from H_(2) and O_(2)via heterogeneous catalysis is an environmentally friendly and atomically economic alternative to the traditional anthraquinone oxidation(AO)process.Optimizing the electronic and geometric structures of the active metals to break the current limitations of hydrogenation rate and H_(2)O_(2)selectivity is a promising and challenging topic.In this study,a series of Pd-Au bimetallic catalysts supported on TiO_(2)with a metal loading of 3.0 wt%and a constant Pd/Au molar ratio(Pd:Au=2:1)were prepared.The catalysts were reduced in H_(2) at different temperatures(473,573 and 673 K),and their catalytic activity for the direct H_(2)O_(2)synthesis were evaluated at 283 K and 0.1MPa.H_(2) reduced Pd-Au catalysts exhibited superior performance in direct H_(2)O_(2)synthesis.The maximum H_(2)O_(2)selectivity of 87.7%and H_(2)O_(2)yield of 3116.4 mmol h^(−1) gPd^(−1) were achieved over the Pd_(2.0)Au_(1.0)-573 catalyst with a H_(2) conversion of 12.8%.The tailored local chemical environment caused by H_(2) reduction creates a balanced ratio of Pd0 and PdO_(x) sites,thus improving the selectivity towards H_(2)O_(2).This work developed an effective strategy for fabrication of highly active and stable Pd-based H_(2)O_(2)synthesis catalysts with high H_(2)O_(2)yield.
基金supported by the Open Funds of Key Laboratory of Functional Inorganic Material Chemistry(Heilongjiang University)Ministry of Education,China.Zheng-Hua Tang acknowledges the funding from Guangdong Natural Science Funds(No.2023A0505050107).
文摘Cu-based nanomaterials have demonstrated great potential for catalyzing the electrosynthesis of oxime compounds,a type of organonitrogen molecule that finds versatile applications in the pharmaceutical industry,medicine production,chemical feedstocks,and other fields.This review first explains the significance of oxime compounds and compares the conventional synthetic approach with the emerging electrochemical method.Then,the Cu-based nanomaterials including Cu-based com-pounds/composites,Cu-based bimetallic alloys,Cu-based high entropy alloys,and Cu-based single-atom catalysts for oxime electrosynthesis are described with some explicit examples to elucidate the structure-performance relationship clearly.Finally,the current challenges and future perspectives of this rapidly developing and evolving field are analyzed with some critical thoughts.This review is anticipated to stimulate more research efforts to be dedicated to this fast-growing yet quite promising field.
基金supported by the Zhejiang Provincial Natural Science Foundation of China(No.LY24B010003)the National Natural Science Foundation of China(No.22102119),and the WenZhou(No.2024R3001).
文摘Transfer hydrogenation(TH)has become the new frontier of hydrogenation science owing to the use of non-H2 hydrogen sources which are safer and easier handling for constructing various hydrogenated products.As for heterogeneous catalysts applied for TH which take advantages of convenient separation and recycling,single-atom catalysts(SACs)are attractive alternatives because of their maximum atom utilization,well-defined active sites and tunable local atomic structure.Recent literature has manifested the good performance of SACs for TH,gaining attention both from academia and industry.In this perspective,we review TH achieved by SACs according to classified hydrogen sources and provide a comprehensive understanding of the relationship between their structural characters and performance for TH.In addition,corresponding synthetic strategies of SACs are also demonstrated to reveal their roles in forming the featured structures.The remained challenges and potential opportunities in this field are also discussed in the end.This review will guide the design of better-performing SACs for TH and give an impetus to the development of green and cost-effective hydrogenation technology.
基金supported by the National Key R&D Program of China(2019YFA0705900 and 2017YFA0204701)the National Natural Science Foundation of China(52225305,22175187,22171273,21905163,and U2032112)the Youth Innovation Promotion Association CAS(2020031).
文摘Acceptor-donor-acceptor(A-D-A)-type nonfullerene acceptors(NFAs)have contributed to an efficiency breakthrough in organic solar cells(OSCs).However,the absence of an in-depth understanding of how to achieve high charge generation probability while guaranteeing low energy loss by molecular design has caused the stagnation of power conversion efficiency(PCE)in A-D-A-type acceptors.The fluorination strategy,as an effective approach to regulating molecular photoelectric and aggregation properties,can significantly affect device performance in OSCs.However,a comprehensive understanding of the relationship between fluorination and photovoltaic performance has been scarcely investigated thus far.Herein,a series of A-D-A-type acceptors,named ZITI-N-nF(n=2,4,6,8,representing the number of fluorine atoms),were designed and synthesized to reveal the underlying work mechanism of OSCs with low energy loss and efficient charge generation via fine-tuning of the charge-transfer state.The results indicate that ZITI-N-6F-based devices exhibit impressive charge generation probability with low energy loss(Eloss)because of the reduced nonradiative recombination,thus leading to a high PCE of 16.11%in binary OSCs and a PCE of 17.09%in ternary OSCs.Notably,a PCE of 16.6%was verified by the National Institute of Metrology,China,which is the highest certified PCE among OSCs based on A-D-A-type NFAs.
