As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an...As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.展开更多
The current collector is a crucial component in lithium-ion batteries and supercapacitor setups,responsible for gathering electrons from electrode materials and directing them into the external circuit.However,as batt...The current collector is a crucial component in lithium-ion batteries and supercapacitor setups,responsible for gathering electrons from electrode materials and directing them into the external circuit.However,as battery systems evolve and the demand for higher energy density increases,the limitations of traditional current collectors,such as high contact resistance and low corrosion resistance,have become increasingly evident.This review investigates the functions and challenges associated with current collectors in modern battery and supercapacitor systems,with a particular focus on using carbon coating methods to enhance their performance.Surface coating,known for its simplicity and wide applicability,emerges as a promising solution to address these challenges.The review provides a comprehensive overview of carbon-coated current collectors across various types of metal and nonmetal substrates in lithium-ion batteries and supercapacitors,including a comparative analysis of coating materials and techniques.It also discusses methods for manufacturing carbon-coated current collectors and their practical implications for the industry.Furthermore,the review explores prospects and opportunities,highlighting the development of next-generation high-performance coatings and emphasizing the importance of advanced current collectors in optimizing energy device performance.展开更多
Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,spec...Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.展开更多
In the research article“Optical Detection of Distal Lung Enzyme Activity in Human Inflammatory Lung Disease”[1],the data availability statement was inadvertently omitted by the publisher.This has now been corrected ...In the research article“Optical Detection of Distal Lung Enzyme Activity in Human Inflammatory Lung Disease”[1],the data availability statement was inadvertently omitted by the publisher.This has now been corrected in the PDF and HTML(full text).展开更多
Objective and Impact Statement.There is a need to develop platforms delineating inflammatory biology of the distal human lung.We describe a platform technology approach to detect in situ enzyme activity and observe dr...Objective and Impact Statement.There is a need to develop platforms delineating inflammatory biology of the distal human lung.We describe a platform technology approach to detect in situ enzyme activity and observe drug inhibition in the distal human lung using a combination of matrix metalloproteinase(MMP)optical reporters,fibered confocal fluorescence microscopy(FCFM),and a bespoke delivery device.Introduction.The development of new therapeutic agents is hindered by the lack of in vivo in situ experimental methodologies that can rapidly evaluate the biological activity or drug-target engagement in patients.Methods.We optimised a novel highly quenched optical molecular reporter of enzyme activity(FIB One)and developed a translational pathway for in-human assessment.Results.We demonstrate the specificity for matrix metalloproteases(MMPs)2,9,and 13 and probe dequenching within physiological levels of MMPs and feasibility of imaging within whole lung models in preclinical settings.Subsequently,in a first-in-human exploratory experimental medicine study of patients with fibroproliferative lung disease,we demonstrate,through FCFM,the MMP activity in the alveolar space measured through FIB One fluorescence increase(with pharmacological inhibition).Conclusion.This translational in situ approach enables a new methodology to demonstrate active drug target effects of the distal lung and consequently may inform therapeutic drug development pathways.展开更多
Aqueous zinc metal batteries(ZMBs)are one of the most promising grid-scale renewable energy storage batteries.However,the practical application of ZMBs is limited by uncontrollable Zn dendrites and parasitic side reac...Aqueous zinc metal batteries(ZMBs)are one of the most promising grid-scale renewable energy storage batteries.However,the practical application of ZMBs is limited by uncontrollable Zn dendrites and parasitic side reactions at the anode interface.Herein,a unique water-confinement hydrogel electrolyte(TONFC/PAM)was constructed by carboxyl-rich nanocellulose(TONFC)and acid amide-rich polyacrylamide(PAM).The parasitic side reactions were effectively suppressed due to limiting the movement of water in the designed hydrogel electrolyte.Meanwhile,the electrostatic interactions with the electron-rich group(-COOH and-CONH2)established fast Zn2+ion transport channels in the electrolyte,enabling an excellent ionic conductivity(30.23 mS cm^(-1))and horizontal deposition of Zn metal.As a result,the Zn||Zn cells and Zn||Cu cells with TONFC/PAM electrolyte achieve a long cycling life of over 1,400 h at 1 mA cm^(-2)and a high average coulombic efficiency of 99.4%,respectively.More importantly,the Zn||MnO2full cells can stably run for 1,000 cycles with a high capacity(~150 mAh g^(-1))at a current density of 2 A g^(-1).These results show that TONFC/PAM is a suitable hydrogel electrolyte for ZMBs,which presents attractive opportunities for future research on ZMBs.展开更多
The development of circularly polarized multiresonant thermally activated delayed fluorescence materials with fast reverse intersystem crossing(RISC)process remains a challenge.Herein,we introduce high-lying excited s...The development of circularly polarized multiresonant thermally activated delayed fluorescence materials with fast reverse intersystem crossing(RISC)process remains a challenge.Herein,we introduce high-lying excited states to assist the RISC process.Through arranging two known MR-TADF emitters tCzBN and DiKTa at the pseudo-ortho position of a chiral skeleton paracyclophane(PCP),the excitedstate density was increased.The proof-of-concept emitter po-PCP-tCzBN-DiKTa shows nearly three times higher kRISC(5.31×10^(4) s^(−1))than PCP-tCzBN(1.73×10^(4) s^(−1))without compromising color purity and exhibiting circularly polarized luminescence with|gPL|values at the 10^(−4) level.The solution-processed organic light-emitting diodes with po-PCP-tCzBNDiKTa show high maximum external quantum efficiency(EQE_(max))reaching 23%with a moderate efficiency roll-off,showing EQE of 18%and 9%at 100 and 1000 cd/m^(2.)展开更多
Investigation of early stages of crystal growth revealed that crystal growth in some systems may not follow the classic route.In the early stages of inorganic crystal growth,precursor molecules and/or nanocrystallites...Investigation of early stages of crystal growth revealed that crystal growth in some systems may not follow the classic route.In the early stages of inorganic crystal growth,precursor molecules and/or nanocrystallites may aggregate into large and disordered particles with the assistance of some polymers or biomolecules.Surface crystallization of these aggregates would then take place to form shells with high crystallinity and density,followed by an extension of the crystallization from surface to core.This so-called reversed crystal growth mechanism has been found in crystallization of several inorganic compounds including zeolites,perovskites,metals and metal oxides,and will be identified in more material systems.The establishment of this new crystal growth route gave us more freedom to control the morphology of crystals and to understand the formation mechanism of many natural minerals.This article gives a brief review of the recent research in this field by featuring some typical examples of the reversed crystal growth.展开更多
Hydrogen is expected to play an important role in future transportation as a promising alternative clean energy source to carbon-based fuels. One of the key challenges to commercialize hydrogen energy is to develop ap...Hydrogen is expected to play an important role in future transportation as a promising alternative clean energy source to carbon-based fuels. One of the key challenges to commercialize hydrogen energy is to develop appropriate onboard hydrogen storage systems, capable of charging and discharging large quantities of hydrogen with fast enough kinetics to meet commercial requirements. Metal organic framework （MOF） is a new type of inorganic and organic hybrid nanoporous particulate materials. Its diverse networks can enhance hydrogen storage through tuning the structure and property of MOFs. The MOF materials so far developed adsorb hydrogen through weak dispersion interactions, which allow significant quantity of hydrogen to be stored at cryogenic temperatures with fast kinetics. Novel MOFs are being developed to strengthen the interactions between hydrogen and MOFs in order to store hydrogen under ambient conditions. This review surveys the development of such candidate materials, their performance and future research needs.展开更多
Arene C(sp^(2))-H bond borylation offers direct and efficient access to aryl boronic esters.Using in situ catalyst activation and photoirradiation,the iron-catalysed C(sp^(2))-H borylation reaction of carboarenes,pyrr...Arene C(sp^(2))-H bond borylation offers direct and efficient access to aryl boronic esters.Using in situ catalyst activation and photoirradiation,the iron-catalysed C(sp^(2))-H borylation reaction of carboarenes,pyrroles,and indoles has been developed using only bench-stable pre-catalysts and reagents.Good functional group tolerance was observed including those not reported using previous methods(ArNH_(2),ArOH,ArSiR_(3),ArP(O)(O)_(2),ArC(O)NR_(2)).Mechanistic studies revealed iron-catalysed reductive deoxygenation,C—F protodefluorination,and a demethylation of aryl methyl ethers by C—O sigma bond hydroboration.展开更多
The electrochemical reduction of CO2 to give CO in the presence of O2 would allow the direct valorization of flue gases from fossil fuel combustion and of CO2 captured from air. However, it is a challenging task becau...The electrochemical reduction of CO2 to give CO in the presence of O2 would allow the direct valorization of flue gases from fossil fuel combustion and of CO2 captured from air. However, it is a challenging task because O2 reduction is thermodynamically favored over that of CO2. 5% O2 in CO2 near catalyst surface is sufficient to completely inhibit the CO2 reduction reaction. Here we report an O2-tolerant catalytic CO2 reduction electrode inspired by part of the natural photosynthesis unit. The electrode comprises of heterogenized cobalt phthalocyanine molecules serving as the cathode catalyst with >95% Faradaic efficiency(FE) for CO2 reduction to CO coated with a polymer of intrinsic microporosity that works as a CO2-selective layer with a CO2/O2 selectivity of $20. Integrated into a flow electrolytic cell, the hybrid electrode operating with a CO2 feed gas containing 5% O2 exhibits a FECOof 75.9% with a total current density of 27.3 mA/cm^2 at a cell voltage of 3.1 V. A FECO of 49.7% can be retained when the O2 fraction increases to 20%. Stable operation for 18 h is demonstrated. The electrochemical performance and O2 tolerance can be further enhanced by introducing cyano and nitro substituents to the phthalocyanine ligand.展开更多
Hydrogen bonding has been employed to suppressnonradiative decay in organic compounds that showroom-temperature phosphorescence (RTP);however, the small number of structurally diverse examplesmakes it unclear how gene...Hydrogen bonding has been employed to suppressnonradiative decay in organic compounds that showroom-temperature phosphorescence (RTP);however, the small number of structurally diverse examplesmakes it unclear how general this strategy is to turnon RTP. In this study, we report highly efficient blueRTP from 4,4′,4′′-nitrilotribenzoic acid (TPA-CO_(2)H)in five structurally and chemically distinct hydrogenbonded supramolecular networks. In doped films inpoly(vinyl alcohol) (PVA), the phosphorescencequantum yield and lifetime (ΦPh and τPh) reach 52%and 275 ms. Boric acid can also be used to turn onRTP, and the performance changes significantlywhen the sample is heated beyond the dehydrationtemperature of this host where there is a 14-foldenhancement in the ΦPh after heat treatment. BlueRTP similar to that observed in PVA was also observed using granulated sugar, gelatine, and paper ashost matrices. This work elucidates for the first timethe role and the generality of hydrogen bonding inactivating efficient blue RTP and examines how thechoice of hydrogen bonding host influences RTPperformance. We further demonstrate how the emission color can be tuned by codoping the films withRhodamine 6G.展开更多
GaSb-based nanowires in a gate-all-around geometry are good candidates for binary p-type transistors,however they require the introduction of compressive strain to enhance the transport properties.Here,we for the firs...GaSb-based nanowires in a gate-all-around geometry are good candidates for binary p-type transistors,however they require the introduction of compressive strain to enhance the transport properties.Here,we for the first time demonstrate epitaxial GaSb-GaASxSb1-x core-shell nanowires with a compressively strained core.Both axial and hydrostatic strain in GaSb core have been measured by X-ray diffraction(XRD)and Raman scattering,respectively.The optimal sample,almost without plastic relaxation,has an axial strain of-0.88%and a hydrostatic strain of-1.46%,leading to a noticeable effect where the light hole band is calculated to be 33.4 meV above the heavy hole band at the T-point.This valence band feature offers more light holes to contribute the transport process,and thus may provide enhanced hole mobility by reducing both the interband scattering and the hole effective mass.Our results show that lattice-mismatched epitaxial core-shell heterostructures of high quality can also be realized in the promising yet demanding GaSb-based system.展开更多
High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that ena...High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that enable us,for the first time,to combine three effective approaches for enhancing the efficiency of nondoped OLEDs.First,the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching.On the other hand,each of the two emitters has two stable conformations in solid films.In their neat films,molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation.One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of“self-doped”neat films.Furthermore,both emitters have relatively high aspect ratios in terms of their molecular shapes.This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical outcoupling.With these three factors,OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100%exciton utilization and deliver over 30%external quantum efficiencies and ultralow efficiency roll-off at high brightness,which have not been observed in reported nondoped OLEDs.展开更多
We have designed and synthesized NaGdF4：Nd^3＋, Yb^3＋, Tm^3＋. magnetic nano- phosphors with combined dual-mode downconversion （DC） and upconversion （UC） photoluminescence upon 800 run excitation. Hexagonal-phas...We have designed and synthesized NaGdF4：Nd^3＋, Yb^3＋, Tm^3＋. magnetic nano- phosphors with combined dual-mode downconversion （DC） and upconversion （UC） photoluminescence upon 800 run excitation. Hexagonal-phase NaGdF4：Nd^3＋, Yb^3＋, Tm^3＋ nanocrystals （NCs） with an average size of 21 nm were synthesized using a solvothermal approach. Nd^3＋, Yb^3＋, Tm^3＋ triple-doped NaGdF4 NCs exhibit a broad range of photoluminescence peaks covering a near infrared first/second window （860-900, 1,000, and 1,060 nm）, and visible emission including blue （475 nm）, green （520 and 542 nm） and yellow （587 nm） after excitation at 800 nm. A mechanism involving circulation of energy over Gd^3＋ sublattices as bridge ions and final trapping by the initial activator ions （Nd^3＋） has been proposed. Penetration depth studies indicate that NIR emission is easily detected even at a large tissue thickness of 10 mm. These paramagnetic nanophosphors demonstrate a large magnetization value of 1.88 emu/g at 20 kOe and longitudinal relaxivity value of 1.2537 mM-1.S-1 as a Tl-weighted magnetic resonance imaging contrast agent. These NaGdF4：Nd^3＋, Yb^3＋ Tm^3＋ NCs are promising for applications in biological and magnetic resonance imaging.展开更多
Chirality or handedness,i.e.,the non-superimposability of a structure(lacking a plane or center of symmetry)with its mirrorimage,strongly impacts various chemistry/biology areas,and plays an important role,e.g.,in mat...Chirality or handedness,i.e.,the non-superimposability of a structure(lacking a plane or center of symmetry)with its mirrorimage,strongly impacts various chemistry/biology areas,and plays an important role,e.g.,in materials chemistry[1].In medicinal chemistry it is critical to evaluate the therapeutic and toxicological properties of all stereoisomers of a drug molecule because diastereoisomers and enantiomers may exhibit distinct biological and pharmacological activities[2].展开更多
The development of high-performance solution-processed red organic light-emitting diodes(OLEDs) remains a challenge,particularly in terms of maintaining efficiency at high luminance. Here, we designed and synthesized ...The development of high-performance solution-processed red organic light-emitting diodes(OLEDs) remains a challenge,particularly in terms of maintaining efficiency at high luminance. Here, we designed and synthesized four novel orange-red thermally activated delayed fluorescence(TADF) dendrimers that are solution-processable: 2GCz BP, 2DPACz BP, 2FBP2GCz and 2FBP2DPACz. We systematically investigated the effect of substitution position and strength of donors on the optoelectronic properties. The reverse intersystem crossing rate constant(kRISC) of the emitters having donors substituted at positions 11and 12 of the dibenzo[a,c]phenazine(BP) is more than 10-times faster than that of compounds substituted having donors substituted at positions 3 and 6. Compound 2DPACz BP, containing stronger donors than 2GCz BP, exhibits a red-shifted emission and smaller singlet-triplet energy splitting, ΔE_(ST), of 0.01 e V. The solution-processed OLED with 10 wt% 2DPACz BP doped in m CP emitted at 640 nm and showed a maximum external quantum efficiency(EQE_(max)) of 7.8%, which was effectively maintained out to a luminance of 1,000 cd m-2. Such a device's performance at relevant display luminance is among the highest for solution-processed red TADF OLEDs. The efficiency of the devices was improved significantly by using 4Cz IPN as an assistant dopant in a hyperfluorescence(HF) configuration, where the 2DPACz BP HF device shows an EQEmaxof 20.0% at λEL of 605 nm and remains high at 11.8% at a luminance of 1,000 cd m-2, which makes this device one of the highest efficiency orange-to-red HF SP-OLEDs to date.展开更多
In an article recently published in Sci.China Chem.,Liao,Jiang,and their co-workers[1]report two N/carbonyl-based multi-resonant thermally activated delayed fluorescence(MR-TADF)emitters,the organic light-emitting dio...In an article recently published in Sci.China Chem.,Liao,Jiang,and their co-workers[1]report two N/carbonyl-based multi-resonant thermally activated delayed fluorescence(MR-TADF)emitters,the organic light-emitting diode(OLED)that uses one of these,MTDMQAO,showed record maximum external quantum efficiencies(EQEmax)for devices using this class of compound.The reason for this impressive device performance stems from a rationale and judicious molecular design,building on a core QAO(aka DiKTa)[2]MR-TADF emitter structure that the authors helped to pioneer[3,4],and decorating a fused derivative of it with an electron-withdrawing triazine unit.展开更多
Zeolitic imidazolate frameworks(ZIFs)are an important subclass of metal-organic frameworks(MOFs)with zeolite-type topology,which can be fabricated under ambient synthesis conditions.However,the applications of ZIFs ar...Zeolitic imidazolate frameworks(ZIFs)are an important subclass of metal-organic frameworks(MOFs)with zeolite-type topology,which can be fabricated under ambient synthesis conditions.However,the applications of ZIFs are commonly limited due to the weak hydrostability of their metal–ligand coordination bonds,particularly under humid and aqueous conditions.In this work,as an example,the hydrolysis behaviours of ZIF-L with a special focus on ZIF-L coatings were tested at aqueous conditions with a wide range of pHs to systematically study and fundamentally understand their structural stability and degradation mechanism.Pristine ZIF-L powder and ZIF-L coatings were severely damaged after only 24 h in aqueous media.Interestingly,the ZIF-L coatings showed two distinct hydrolyzation pathways regardless of pH conditions,exhibiting either a ring-shaped etching or unfolding behaviours.While the ZIF-L powders were hydrolyzed almost identically across all pH conditions.With this new understanding,a facile silk fibroin(SF)protein modification method was developed to enhance the hydrostability of ZIF-L coatings in aqueous media.The effect of protein concentration on surface coating was systemically studied.ZIF-L coating retained its surface morphology after soaking in water and demonstrated switchable super wetting properties and superior separation performance for oil/water mixture.As a result,the quick SF protein modification significantly enhanced the stability of ZIF-L coatings under various pHs,while retaining their switchable wetting property and excellent separation performance.展开更多
基金supported by Chinese Academy of Sciences(Grant No.2018PS0011)100 Talent Plan of Chinese Academy of Sciences+4 种基金Natural Science Foundation of China(Grant No.61971405)the Department of Science and Technology(GoI)for support through the Project Nos.DST FILE NO.YSS/2015/001712,DST 11-IFAPH-07 and DST FILE NO.DST/TMD/SERI/HUBthe financial support from Equipment Research Program(Grant No.6140721050215)the Ontario Ministry of Research and Innovation(ER15-11-123)the Natural Science and Engineering Council of Canada(RGPIN-2019-05994).
文摘As sustainable energy becomes a major concern for modern society,renewable and clean energy systems need highly active,stable,and low-cost catalysts for the oxygen evolution reaction(OER).Mesoporous materials offer an attractive route for generating efficient electrocatalysts with high mass transport capabilities.Herein,we report an efficient hard templating pathway to design and synthesize three-dimensional(3-D)mesoporous ternary nickel iron nitride(Ni3FeN).The as-synthesized electrocatalyst shows good OER performance in an alkaline solution with low overpotential(259 mV)and a small Tafel slope(54 mV dec?1),giving superior performance to IrO2 and RuO2 catalysts.The highly active contact area,the hierarchical porosity,and the synergistic effect of bimetal atoms contributed to the improved electrocatalytic performance toward OER.In a practical rechargeable Zn–air battery,mesoporous Ni3FeN is also shown to deliver a lower charging voltage and longer lifetime than RuO2.This work opens up a new promising approach to synthesize active OER electrocatalysts for energy-related devices.
基金Innovate UK:Coated current collector for battery performance improvement,Grant/Award Numbers:CONTACT,ref/10041084,2023-2025Innovate UK:Thin and lightweight current collector for lithium-ion battery,Grant/Award Numbers:CONDUCTOR,ref/10047927+3 种基金EPSRC First Grant:Energy storage electrode manufacture,Grant/Award Number:EP/P026818/1EPSRC Industrial Strategy:3D electrodes from 2D materials,Grant/Award Number:EP/R023034/1Innovate UK:Scalable electrophoretic manufacture of highdensity two-dimensional materials for energy storage applications,Grant/Award Number:ref/132508Innovate UK:Current collector for improved battery performance COATED,Grant/Award Numbers:ref/2021,2022,98297。
文摘The current collector is a crucial component in lithium-ion batteries and supercapacitor setups,responsible for gathering electrons from electrode materials and directing them into the external circuit.However,as battery systems evolve and the demand for higher energy density increases,the limitations of traditional current collectors,such as high contact resistance and low corrosion resistance,have become increasingly evident.This review investigates the functions and challenges associated with current collectors in modern battery and supercapacitor systems,with a particular focus on using carbon coating methods to enhance their performance.Surface coating,known for its simplicity and wide applicability,emerges as a promising solution to address these challenges.The review provides a comprehensive overview of carbon-coated current collectors across various types of metal and nonmetal substrates in lithium-ion batteries and supercapacitors,including a comparative analysis of coating materials and techniques.It also discusses methods for manufacturing carbon-coated current collectors and their practical implications for the industry.Furthermore,the review explores prospects and opportunities,highlighting the development of next-generation high-performance coatings and emphasizing the importance of advanced current collectors in optimizing energy device performance.
基金This study was supported by the National Nat-ural Science Foundation of China(No.22379105)the Natural Sci-ence Foundation of Shanxi Province(Nos.20210302123110 and 202303021211059)the Open Fund Project of Ningxia Sinostar Display Material Co.,Ltd.
文摘Although doped hole-transport materials(HTMs)off er an effi ciency benefi t for perovskite solar cells(PSCs),they inevi-tably diminish the stability.Here,we describe the use of various chlorinated small molecules,specifi cally fl uorenone-triphenylamine(FO-TPA)-x-Cl[x=para,meta,and ortho(p,m,and o)],with diff erent chlorine-substituent positions,as dopant-free HTMs for PSCs.These chlorinated molecules feature a symmetrical donor-acceptor-donor structure and ideal intramolecular charge transfer properties,allowing for self-doping and the establishment of built-in potentials for improving charge extraction.Highly effi cient hole-transfer interfaces are constructed between perovskites and these HTMs by strategi-cally modifying the chlorine substitution.Thus,the chlorinated HTM-derived inverted PSCs exhibited superior effi ciencies and air stabilities.Importantly,the dopant-free HTM FO-TPA-o-Cl not only attains a power conversion effi ciency of 20.82% but also demonstrates exceptional stability,retaining 93.8%of its initial effi ciency even after a 30-day aging test conducted under ambient air conditions in PSCs without encapsulation.These fi ndings underscore the critical role of chlorine-substituent regulation in HTMs in ensuring the formation and maintenance of effi cient and stable PSCs.
文摘In the research article“Optical Detection of Distal Lung Enzyme Activity in Human Inflammatory Lung Disease”[1],the data availability statement was inadvertently omitted by the publisher.This has now been corrected in the PDF and HTML(full text).
基金supported by the Medical Research Council(under the Developmental Pathway Funding Scheme grant number MR/J014702)the Engineering and Physical Sciences Research Council(EP/K03197X/1,EP/R005257/1,and NS/A000049/1)+3 种基金the Wellcome Trust(203148/Z/16/Z)AA is supported by a Cancer Research UK Clinician Scientist Fellowship(A24867)TV is supported by a Medtronic/Royal Academy of Engineering Research Chair(RCSRF1819\7\34)The research leading to these results has received funding from the European Union Seventh Framework Programme FP72012 under grant agreement No.326465(AMF).
文摘Objective and Impact Statement.There is a need to develop platforms delineating inflammatory biology of the distal human lung.We describe a platform technology approach to detect in situ enzyme activity and observe drug inhibition in the distal human lung using a combination of matrix metalloproteinase(MMP)optical reporters,fibered confocal fluorescence microscopy(FCFM),and a bespoke delivery device.Introduction.The development of new therapeutic agents is hindered by the lack of in vivo in situ experimental methodologies that can rapidly evaluate the biological activity or drug-target engagement in patients.Methods.We optimised a novel highly quenched optical molecular reporter of enzyme activity(FIB One)and developed a translational pathway for in-human assessment.Results.We demonstrate the specificity for matrix metalloproteases(MMPs)2,9,and 13 and probe dequenching within physiological levels of MMPs and feasibility of imaging within whole lung models in preclinical settings.Subsequently,in a first-in-human exploratory experimental medicine study of patients with fibroproliferative lung disease,we demonstrate,through FCFM,the MMP activity in the alveolar space measured through FIB One fluorescence increase(with pharmacological inhibition).Conclusion.This translational in situ approach enables a new methodology to demonstrate active drug target effects of the distal lung and consequently may inform therapeutic drug development pathways.
基金supported by the National Natural Science Foundation of China(22209140,52202286)the Natural Science Foundation of Shandong Province(ZR2022QE059)+5 种基金the Shandong Laboratory of Advanced Materials and Green Manufacturing at Yantai(AMGM2023A08)the Natural Science Foundation of Zhejiang Province(LQ23B030011,LY24B030006)the Scientific Research Fund of Zhejiang Provincial Education Department(Y202148249)Science and Technology Plan Project of Wenzhou Municipality(ZG2024055)Wenzhou Association for Science and Technology Innovation Program(NLTS2024-013)the Basic Research Project of Wenzhou City(G20220016)。
文摘Aqueous zinc metal batteries(ZMBs)are one of the most promising grid-scale renewable energy storage batteries.However,the practical application of ZMBs is limited by uncontrollable Zn dendrites and parasitic side reactions at the anode interface.Herein,a unique water-confinement hydrogel electrolyte(TONFC/PAM)was constructed by carboxyl-rich nanocellulose(TONFC)and acid amide-rich polyacrylamide(PAM).The parasitic side reactions were effectively suppressed due to limiting the movement of water in the designed hydrogel electrolyte.Meanwhile,the electrostatic interactions with the electron-rich group(-COOH and-CONH2)established fast Zn2+ion transport channels in the electrolyte,enabling an excellent ionic conductivity(30.23 mS cm^(-1))and horizontal deposition of Zn metal.As a result,the Zn||Zn cells and Zn||Cu cells with TONFC/PAM electrolyte achieve a long cycling life of over 1,400 h at 1 mA cm^(-2)and a high average coulombic efficiency of 99.4%,respectively.More importantly,the Zn||MnO2full cells can stably run for 1,000 cycles with a high capacity(~150 mAh g^(-1))at a current density of 2 A g^(-1).These results show that TONFC/PAM is a suitable hydrogel electrolyte for ZMBs,which presents attractive opportunities for future research on ZMBs.
基金the China Scholarship Council(grant no.202106310038)for supportsupport from the China Postdoctoral Science Foundation(grant no.2022TQ0227)+2 种基金the Natural Science Foundation of Jiangsu Province,China(grant no.BK20230508)the China Scholarship Council(grant no.201906250199)support from the National Natural Science Foundation of China(grant no.52130304)the Suzhou Key Laboratory of Functional Nano&Soft Materials,the Collaborative Innovation Center of Suzhou Nano Science&Technology,the 111 Project.
文摘The development of circularly polarized multiresonant thermally activated delayed fluorescence materials with fast reverse intersystem crossing(RISC)process remains a challenge.Herein,we introduce high-lying excited states to assist the RISC process.Through arranging two known MR-TADF emitters tCzBN and DiKTa at the pseudo-ortho position of a chiral skeleton paracyclophane(PCP),the excitedstate density was increased.The proof-of-concept emitter po-PCP-tCzBN-DiKTa shows nearly three times higher kRISC(5.31×10^(4) s^(−1))than PCP-tCzBN(1.73×10^(4) s^(−1))without compromising color purity and exhibiting circularly polarized luminescence with|gPL|values at the 10^(−4) level.The solution-processed organic light-emitting diodes with po-PCP-tCzBNDiKTa show high maximum external quantum efficiency(EQE_(max))reaching 23%with a moderate efficiency roll-off,showing EQE of 18%and 9%at 100 and 1000 cd/m^(2.)
文摘Investigation of early stages of crystal growth revealed that crystal growth in some systems may not follow the classic route.In the early stages of inorganic crystal growth,precursor molecules and/or nanocrystallites may aggregate into large and disordered particles with the assistance of some polymers or biomolecules.Surface crystallization of these aggregates would then take place to form shells with high crystallinity and density,followed by an extension of the crystallization from surface to core.This so-called reversed crystal growth mechanism has been found in crystallization of several inorganic compounds including zeolites,perovskites,metals and metal oxides,and will be identified in more material systems.The establishment of this new crystal growth route gave us more freedom to control the morphology of crystals and to understand the formation mechanism of many natural minerals.This article gives a brief review of the recent research in this field by featuring some typical examples of the reversed crystal growth.
文摘Hydrogen is expected to play an important role in future transportation as a promising alternative clean energy source to carbon-based fuels. One of the key challenges to commercialize hydrogen energy is to develop appropriate onboard hydrogen storage systems, capable of charging and discharging large quantities of hydrogen with fast enough kinetics to meet commercial requirements. Metal organic framework （MOF） is a new type of inorganic and organic hybrid nanoporous particulate materials. Its diverse networks can enhance hydrogen storage through tuning the structure and property of MOFs. The MOF materials so far developed adsorb hydrogen through weak dispersion interactions, which allow significant quantity of hydrogen to be stored at cryogenic temperatures with fast kinetics. Novel MOFs are being developed to strengthen the interactions between hydrogen and MOFs in order to store hydrogen under ambient conditions. This review surveys the development of such candidate materials, their performance and future research needs.
基金S.P.T.thanks The Royal Society for a University Research Fel-lowship(RF191015)J.H.D.and S.P.T.acknowledge GSK and EPSRC(110002)The Royal Society(RF191015)for postdoctoral funding.L.B.acknowledges The Royal Society and The University of Edinburgh for a Ph.D.studentship(RF191015).
文摘Arene C(sp^(2))-H bond borylation offers direct and efficient access to aryl boronic esters.Using in situ catalyst activation and photoirradiation,the iron-catalysed C(sp^(2))-H borylation reaction of carboarenes,pyrroles,and indoles has been developed using only bench-stable pre-catalysts and reagents.Good functional group tolerance was observed including those not reported using previous methods(ArNH_(2),ArOH,ArSiR_(3),ArP(O)(O)_(2),ArC(O)NR_(2)).Mechanistic studies revealed iron-catalysed reductive deoxygenation,C—F protodefluorination,and a demethylation of aryl methyl ethers by C—O sigma bond hydroboration.
基金supported by the U.S. National Science Foundation (CHE-1651717)the Croucher Fellowship for Postdoctoral Research+1 种基金supported by Global Innovation Initiative from Institute of International Educationsupport from Shenzhen Fundamental Research Funding (JCYJ20160608140827794)
文摘The electrochemical reduction of CO2 to give CO in the presence of O2 would allow the direct valorization of flue gases from fossil fuel combustion and of CO2 captured from air. However, it is a challenging task because O2 reduction is thermodynamically favored over that of CO2. 5% O2 in CO2 near catalyst surface is sufficient to completely inhibit the CO2 reduction reaction. Here we report an O2-tolerant catalytic CO2 reduction electrode inspired by part of the natural photosynthesis unit. The electrode comprises of heterogenized cobalt phthalocyanine molecules serving as the cathode catalyst with >95% Faradaic efficiency(FE) for CO2 reduction to CO coated with a polymer of intrinsic microporosity that works as a CO2-selective layer with a CO2/O2 selectivity of $20. Integrated into a flow electrolytic cell, the hybrid electrode operating with a CO2 feed gas containing 5% O2 exhibits a FECOof 75.9% with a total current density of 27.3 mA/cm^2 at a cell voltage of 3.1 V. A FECO of 49.7% can be retained when the O2 fraction increases to 20%. Stable operation for 18 h is demonstrated. The electrochemical performance and O2 tolerance can be further enhanced by introducing cyano and nitro substituents to the phthalocyanine ligand.
基金S.W.thanks the China Scholarship Council(grant no.201906250199)for supportfunding from the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie grant agreement No.897098(AIERTP-PLED)+1 种基金support from the Marie Skłodowska-Curie Individual FellowshipWe also thank the United Kingdom’s Engineering and Physical Sciences Research Council for support(grant no.EP/W007517/1).
文摘Hydrogen bonding has been employed to suppressnonradiative decay in organic compounds that showroom-temperature phosphorescence (RTP);however, the small number of structurally diverse examplesmakes it unclear how general this strategy is to turnon RTP. In this study, we report highly efficient blueRTP from 4,4′,4′′-nitrilotribenzoic acid (TPA-CO_(2)H)in five structurally and chemically distinct hydrogenbonded supramolecular networks. In doped films inpoly(vinyl alcohol) (PVA), the phosphorescencequantum yield and lifetime (ΦPh and τPh) reach 52%and 275 ms. Boric acid can also be used to turn onRTP, and the performance changes significantlywhen the sample is heated beyond the dehydrationtemperature of this host where there is a 14-foldenhancement in the ΦPh after heat treatment. BlueRTP similar to that observed in PVA was also observed using granulated sugar, gelatine, and paper ashost matrices. This work elucidates for the first timethe role and the generality of hydrogen bonding inactivating efficient blue RTP and examines how thechoice of hydrogen bonding host influences RTPperformance. We further demonstrate how the emission color can be tuned by codoping the films withRhodamine 6G.
基金This work was supported by the Swedish Research Council(VR)the Swedish Foundation for Strategic Research(SSF).
文摘GaSb-based nanowires in a gate-all-around geometry are good candidates for binary p-type transistors,however they require the introduction of compressive strain to enhance the transport properties.Here,we for the first time demonstrate epitaxial GaSb-GaASxSb1-x core-shell nanowires with a compressively strained core.Both axial and hydrostatic strain in GaSb core have been measured by X-ray diffraction(XRD)and Raman scattering,respectively.The optimal sample,almost without plastic relaxation,has an axial strain of-0.88%and a hydrostatic strain of-1.46%,leading to a noticeable effect where the light hole band is calculated to be 33.4 meV above the heavy hole band at the T-point.This valence band feature offers more light holes to contribute the transport process,and thus may provide enhanced hole mobility by reducing both the interband scattering and the hole effective mass.Our results show that lattice-mismatched epitaxial core-shell heterostructures of high quality can also be realized in the promising yet demanding GaSb-based system.
基金National Natural Science Foundation of China,Grant/Award Numbers:51821002,52003185,52003186,52130304National Key Research&Development Program of China,Grant/Award Numbers:2020YFA0714601,2020YFA0714604+2 种基金Suzhou Key Laboratory of Functional Nano&Soft MaterialsCollaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Project。
文摘High-performance nondoped organic light-emitting diodes(OLEDs)are promising technologies for future commercial applications.Herein,we synthesized two new thermally activated delayed fluorescence(TADF)emitters that enable us,for the first time,to combine three effective approaches for enhancing the efficiency of nondoped OLEDs.First,the two emitters are designed to have high steric hindrances such that their emitting cores will be suitably isolated from those of their neighbors to minimize concentration quenching.On the other hand,each of the two emitters has two stable conformations in solid films.In their neat films,molecules with the minority conformation behave effectively as dopants in the matrix composing of the majority conformation.One hundred percent exciton harvesting is thus theoretically feasible in this unique architecture of“self-doped”neat films.Furthermore,both emitters have relatively high aspect ratios in terms of their molecular shapes.This leads to films with preferred molecular orientations enabling high populations of horizontal dipoles beneficial for optical outcoupling.With these three factors,OLEDs with nondoped emitting layers of the respective emitters both achieve nearly 100%exciton utilization and deliver over 30%external quantum efficiencies and ultralow efficiency roll-off at high brightness,which have not been observed in reported nondoped OLEDs.
文摘We have designed and synthesized NaGdF4：Nd^3＋, Yb^3＋, Tm^3＋. magnetic nano- phosphors with combined dual-mode downconversion （DC） and upconversion （UC） photoluminescence upon 800 run excitation. Hexagonal-phase NaGdF4：Nd^3＋, Yb^3＋, Tm^3＋ nanocrystals （NCs） with an average size of 21 nm were synthesized using a solvothermal approach. Nd^3＋, Yb^3＋, Tm^3＋ triple-doped NaGdF4 NCs exhibit a broad range of photoluminescence peaks covering a near infrared first/second window （860-900, 1,000, and 1,060 nm）, and visible emission including blue （475 nm）, green （520 and 542 nm） and yellow （587 nm） after excitation at 800 nm. A mechanism involving circulation of energy over Gd^3＋ sublattices as bridge ions and final trapping by the initial activator ions （Nd^3＋） has been proposed. Penetration depth studies indicate that NIR emission is easily detected even at a large tissue thickness of 10 mm. These paramagnetic nanophosphors demonstrate a large magnetization value of 1.88 emu/g at 20 kOe and longitudinal relaxivity value of 1.2537 mM-1.S-1 as a Tl-weighted magnetic resonance imaging contrast agent. These NaGdF4：Nd^3＋, Yb^3＋ Tm^3＋ NCs are promising for applications in biological and magnetic resonance imaging.
基金the financial support from the National Natural Science Foundation of China(21772151)Natural Science Foundation of Hubei Province(2018CFA084)。
文摘Chirality or handedness,i.e.,the non-superimposability of a structure(lacking a plane or center of symmetry)with its mirrorimage,strongly impacts various chemistry/biology areas,and plays an important role,e.g.,in materials chemistry[1].In medicinal chemistry it is critical to evaluate the therapeutic and toxicological properties of all stereoisomers of a drug molecule because diastereoisomers and enantiomers may exhibit distinct biological and pharmacological activities[2].
基金the China Scholarship Council(201806890001)support from the Royal Academy of Engineering Enterprise Fellowship (EF2122-13106)EPSRC (EP/W015137/1, EP/W524505/1) for financial support。
文摘The development of high-performance solution-processed red organic light-emitting diodes(OLEDs) remains a challenge,particularly in terms of maintaining efficiency at high luminance. Here, we designed and synthesized four novel orange-red thermally activated delayed fluorescence(TADF) dendrimers that are solution-processable: 2GCz BP, 2DPACz BP, 2FBP2GCz and 2FBP2DPACz. We systematically investigated the effect of substitution position and strength of donors on the optoelectronic properties. The reverse intersystem crossing rate constant(kRISC) of the emitters having donors substituted at positions 11and 12 of the dibenzo[a,c]phenazine(BP) is more than 10-times faster than that of compounds substituted having donors substituted at positions 3 and 6. Compound 2DPACz BP, containing stronger donors than 2GCz BP, exhibits a red-shifted emission and smaller singlet-triplet energy splitting, ΔE_(ST), of 0.01 e V. The solution-processed OLED with 10 wt% 2DPACz BP doped in m CP emitted at 640 nm and showed a maximum external quantum efficiency(EQE_(max)) of 7.8%, which was effectively maintained out to a luminance of 1,000 cd m-2. Such a device's performance at relevant display luminance is among the highest for solution-processed red TADF OLEDs. The efficiency of the devices was improved significantly by using 4Cz IPN as an assistant dopant in a hyperfluorescence(HF) configuration, where the 2DPACz BP HF device shows an EQEmaxof 20.0% at λEL of 605 nm and remains high at 11.8% at a luminance of 1,000 cd m-2, which makes this device one of the highest efficiency orange-to-red HF SP-OLEDs to date.
文摘In an article recently published in Sci.China Chem.,Liao,Jiang,and their co-workers[1]report two N/carbonyl-based multi-resonant thermally activated delayed fluorescence(MR-TADF)emitters,the organic light-emitting diode(OLED)that uses one of these,MTDMQAO,showed record maximum external quantum efficiencies(EQEmax)for devices using this class of compound.The reason for this impressive device performance stems from a rationale and judicious molecular design,building on a core QAO(aka DiKTa)[2]MR-TADF emitter structure that the authors helped to pioneer[3,4],and decorating a fused derivative of it with an electron-withdrawing triazine unit.
基金supported by start-up funding from the School of Engineering,at the University of Edinburgh.
文摘Zeolitic imidazolate frameworks(ZIFs)are an important subclass of metal-organic frameworks(MOFs)with zeolite-type topology,which can be fabricated under ambient synthesis conditions.However,the applications of ZIFs are commonly limited due to the weak hydrostability of their metal–ligand coordination bonds,particularly under humid and aqueous conditions.In this work,as an example,the hydrolysis behaviours of ZIF-L with a special focus on ZIF-L coatings were tested at aqueous conditions with a wide range of pHs to systematically study and fundamentally understand their structural stability and degradation mechanism.Pristine ZIF-L powder and ZIF-L coatings were severely damaged after only 24 h in aqueous media.Interestingly,the ZIF-L coatings showed two distinct hydrolyzation pathways regardless of pH conditions,exhibiting either a ring-shaped etching or unfolding behaviours.While the ZIF-L powders were hydrolyzed almost identically across all pH conditions.With this new understanding,a facile silk fibroin(SF)protein modification method was developed to enhance the hydrostability of ZIF-L coatings in aqueous media.The effect of protein concentration on surface coating was systemically studied.ZIF-L coating retained its surface morphology after soaking in water and demonstrated switchable super wetting properties and superior separation performance for oil/water mixture.As a result,the quick SF protein modification significantly enhanced the stability of ZIF-L coatings under various pHs,while retaining their switchable wetting property and excellent separation performance.
