We propose a simple embedding method for computing the eigenvalues and eigenfunctions of the Laplace-Beltrami operator on implicit surfaces.The approach follows an embedding approach for solving the surface eikonal eq...We propose a simple embedding method for computing the eigenvalues and eigenfunctions of the Laplace-Beltrami operator on implicit surfaces.The approach follows an embedding approach for solving the surface eikonal equation.We replace the differential operator on the interface with a typical Cartesian differential operator in the surface neighborhood.Our proposed algorithm is easy to implement and efficient.We will give some two-and three-dimensional numerical examples to demonstrate the effectiveness of our proposed approach.展开更多
At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active si...At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets(Zn/NC NSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH_(3)rate and Faradaic efficiencies after multiple cycles.The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N_(4)sites in the catalyst.DFT calculation confirms that Zn/NC with Zn-N_(4)configuration has a lower energy barrier for the formation of^(*)NNH intermediate compared with pure N-doped carbon nanosheets(N-C NSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.展开更多
Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrain...Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrained by critical challenges,including dendrites,water-induced hydrogen evolution,and passivation.In this study,a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method.The ultrathin interphase layer(~1μm)is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1Å,which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions,contributing to a uniform and highly reversible zinc deposition.With the shielding of the interphase layer,an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and~700 h at 1 mA cm^(−2),far exceeding that of the bare zinc anodes(250 and 70 h).Furthermore,as a proof-of-concept demonstration,the full cell paired with MnO_(2) cathode demonstrates improved rate performances and stable cycling(1200 cycles at 1 A g−1).This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.展开更多
Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices....Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices.In this paper,we introduce a 2.5μm-thick asymmetric and ultrastrong separator,which can induce tissue-like lithium deposits.The asymmetric separator,denoted by utPE@Cu_(2)O,was prepared by selective synthesis of Cu_(2)O nanoparticles on one of the outer surfaces of a nanofibrous(diameter~10 nm)ultrastrong ultrahigh molecular weight polyethylene(UHMWPE)membrane.Microscopic analysis shows that the lithium deposits have tissue-like morphology,resulting in the symmetric lithium cells assembled using utPE@Cu_(2)O with symmetric Cu_(2)O coating exhibiting stable performance for over 2000 h of cycling.This work demonstrates the feasibility of a facile approach ultrathin separators for the deployment of lithium metal batteries,providing a pathway towards enhanced battery performance and safety.展开更多
Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caus...Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.展开更多
With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices....With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.展开更多
Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum s...Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum solvation model to predict the reaction energetics of NO3RR on pure copper surface in alkaline media.The potential-dependent mechanism on the most prevailing Cu(111)and the minor(100)and(110)facets were established,in consideration of NO_(2)_(−),NO,NH_(3),NH_(2)OH,N_(2),and N_(2)O as the main products.The computational results show that the major Cu(111)is the ideal surface to produce ammonia with the highest onset potential at 0.06 V(until−0.37 V)and the highest optimal potential at−0.31 V for ammonia production without kinetic obstacles in activation energies at critical steps.For other minor facets,the secondary Cu(100)shows activity to ammonia from−0.03 to−0.54 V with the ideal potential at−0.50 V,which requires larger overpotential to overcome kinetic activation energy barriers.The least Cu(110)possesses the longest potential range for ammonia yield from−0.27 to−1.12 V due to the higher adsorption coverage of nitrate,but also with higher tendency to generate di-nitrogen species.Experimental evaluations on commercial Cu/C electrocatalyst validated the accuracy of our proposed mechanism.The most influential(111)surface with highest percentage in electrocatalyst determined the trend of ammonia production.In specific,the onset potential of ammonia production at 0.1 V and emergence of yield rate peak at−0.3 V in experiments precisely located in the predicted potentials on Cu(111).Four critical factors for the high ammonia yield and selectivity on Cu surface via NO3RR are summarized,including high NO3RR activity towards ammonia on the dominant Cu(111)facet,more possibilities to produce ammonia along different pathways on each facet,excellent ability for HER inhibition and suitable surface size to suppress di-nitrogen species formation at high nitrate coverage.Overall,our work provides comprehensive potential-dependent insights into the reaction details of NO3RR to ammonia,which can serve as references for the future development of NO3RR electrocatalysts,achieving higher activity and selectivity by maximizing these characteristics of copper-based materials.展开更多
Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabrica...Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabricate portable glucose sensors by recycling copper from e-waste.We bring up a laser-induced full-automatic fabrication method for synthesizing continuous heterogeneous Cu_(x)O(h-Cu_(x)O)nano-skeletons electrode for glucose sensing,offering rapid(<1 min),clean,air-compatible,and continuous fabrication,applicable to a wide range of Cu-containing substrates.Leveraging this approach,h-Cu_(x)O nanoskeletons,with an inner core predominantly composed of Cu_(2)O with lower oxygen content,juxtaposed with an outer layer rich in amorphous Cu_(x)O(a-Cu_(x)O)with higher oxygen content,are derived from discarded printed circuit boards.When employed in glucose detection,the h-Cu_(x)O nano-skeletons undergo a structural evolution process,transitioning into rigid Cu_(2)O@CuO nano-skeletons prompted by electrochemical activation.This transformation yields exceptional glucose-sensing performance(sensitivity:9.893 mA mM^(-1) cm^(-2);detection limit:0.34μM),outperforming most previously reported glucose sensors.Density functional theory analysis elucidates that the heterogeneous structure facilitates gluconolactone desorption.This glucose detection device has also been downsized to optimize its scalability and portability for convenient integration into people’s everyday lives.展开更多
Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7...Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7−δ)(SF)exhibits superior proton uptake and rapid ionic conduction,boosting activity.However,excessive proton uptake during RePCC operation degrades SF’s crystal structure,impacting durability.This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes,incorporating Sr-deficiency and Nb-substitution to create Sr_(2.8)Fe_(1.8)Nb_(0.2)O_(7−δ)(D-SFN).Nb stabilizes SF’s crystal,curbing excessive phase formation,and Sr-deficiency boosts oxygen vacancy concentration,optimizing oxygen transport.The D-SFN electrode demonstrates outstanding activity and durability,achieving a peak power density of 596 mW cm^(−2)in fuel cell mode and a current density of−1.19 A cm^(−2)in electrolysis mode at 1.3 V,650℃,with excellent cycling durability.This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage.展开更多
Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport...Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.展开更多
Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)...Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.展开更多
Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the ...Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.展开更多
Close-space sublimation(CSS)has been demonstrated as an alternative vacuum deposition technique for fabricating organic light-emitting diodes(OLEDs).CSS utilizes a planar donor plate pre-coated with organic thin films...Close-space sublimation(CSS)has been demonstrated as an alternative vacuum deposition technique for fabricating organic light-emitting diodes(OLEDs).CSS utilizes a planar donor plate pre-coated with organic thin films as an area source to rapidly transfer the donor film to a device substrate at temperatures below 200℃.CSS is also conformal and capable of depositing on odd-shaped substrates using flexible donor media.The evaporation behaviors of organic donor films under CSS were fully characterized using model OLED materials and CSS-deposited films exhibited comparable device performances in an OLED stack to films deposited by conventional point sources.The low temperature and conformal nature of CSS,along with its high material utilization and short process time,make it a promising method for fabricating flexible OLED displays.展开更多
Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfac...Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene(NG)on SiC(NG@SiC).This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction,making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration.Both density functional theory(DFT)analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds,enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation.As a proof-of-concept study,this well-designed NG@SiC anode shows good reversible capacity(1197.5 mAh g^(−1)after 200 cycles at 0.1 A g^(−1))and cycling durability with 76.6%capacity retention at 447.8 mAh g^(−1)after 1000 cycles at 10.0 A g^(−1).As expected,the lithium-ion full cell(LiFePO_(4)/C//NG@SiC)shows superior rate capability and cycling stability.This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond.展开更多
The high-density,vertically aligned retinal neuron array provides effective vision,a feature we aim to replicate with electronic devices.However,the conventional complementary metal-oxide-semiconductor(CMOS)image sens...The high-density,vertically aligned retinal neuron array provides effective vision,a feature we aim to replicate with electronic devices.However,the conventional complementary metal-oxide-semiconductor(CMOS)image sensor,based on separate designs for sensing,memory,and processing units,limits its integration density.Moreover,redundant signal communication significantly increases energy consumption.Current neuromorphic devices integrating sensing and signal processing show promise in various computer vision applications,but there is still a need for frame-based imaging with good compatibility.In this study,we developed a dual-mode image sensor based on a high-density all-inorganic perovskite nanowire array.The device can switch between frame-based standard imaging mode and neuromorphic imaging mode by applying different biases.This unique bias-dependent photo response is based on a well-designed energy band diagram.The biomimetic alignment of nanowires ensures the potential for high-resolution imaging.To further demonstrate the imaging ability,we conducted pattern reconstruction in both modes with a 10×10 crossbar device.This study introduces a novel image sensor with high compatibility and efficiency,suitable for various applications including computer vision,surveillance,and robotics.展开更多
Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,ach...Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,achieving higher than 26%power conversion efficiency to date.These materials have potential to be deployed for many other applications beyond photovoltaics like photodetectors,sensors,light-emitting diodes(LEDs),and resistors.To address the looming challenge of Moore’s law and the Von Neumann bottleneck,many new technologies regarding the computation of architectures and storage of information are being extensively researched.Since the discovery of the memristor as a fourth component of the circuit,many materials are explored for memristive applications.Lately,researchers have advanced the exploration of OHPs for memristive applications.These materials possess promising memristive properties and various kinds of halide perovskites have been used for different applications that are not only limited to data storage but expand towards artificial synapses,and neuromorphic computing.Herein we summarize the recent advancements of OHPs for memristive applications,their unique electronic properties,fabrication of materials,and current progress in this field with some future perspectives and outlooks.展开更多
Rechargeable aprotic Li-O_(2)batteries have attractea increasing attention due to their extremely high capacity,and it is very important to design appropriate strategies to synthesize efficient catalysts used as oxyge...Rechargeable aprotic Li-O_(2)batteries have attractea increasing attention due to their extremely high capacity,and it is very important to design appropriate strategies to synthesize efficient catalysts used as oxygen cathode.In present work,we present an expedient "instantaneous nucleation and epitaxial growth"(INEG) synthesis strategy for convenient and large-scale synthesis of ultrafine MOCPs nanoparticles(size 50-100 nm) with obvious advantages such as fast synthesis,high yields,low costs and reduced synthetic steps.The bimetallic Ru/Co-MOCPs are further pyrolyzed to obtain bimetallic Coand low content of Ru-based nanoparticles embedded within nitrogen-doped carbon(Ru/Co@N-C) as an efficient catalyst used in Li-O_(2)battery.The Ru/Co@N-C provides porous carbon framework for the ion transportation and O_(2)diffusion,and has large amounts of metal/nonmetal sites as active site to promote the oxygen reduction reaction(ORR)/oxygen evolution reaction(OER) in Li-O_(2)batteries.As a consequence,a high discharge specific capacity of 15246 mA h g^(-1)at 250 mA g^(-1), excellent rate capability at different current densities,and stable overpotential during cycling,are achieved.This work opened up a new understanding for the industrialized synthesis of ultrafine catalysts for Li-O_(2)batteries with excellent structural characteristics and electrochemical performance.展开更多
Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified ...Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified by cetyltrimethylammonium bromide(CTAB) and trimethoxy(3,3,4,4,5,5,6,6,7,7,8,8,8-trideca fluorooctyl) silane(FOTS) to increase the hydrophobicity of MXenes.The ammonia(NH_(3)) production rate and faradaic efficiency(FE) are improved from 37.62 to 54.01 μg h^(-1)mg_(cat)^(-1).and 5.5% to 18.1% at-0.7 V vs.RHE,respectively after surface modification.^(15)N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N_(2) in the electrolyte.The excellent NRR activity of surface hydrophobic MXenes is mainly due to surfactant molecules,which inhibit the entry of water molecules and the competitive HER,which have been verified by in situ FT-IR,DFT and molecular dynamics calculations.This strategy provides an ingenious method to design more active NRR electrocatalysts.展开更多
基金supported in part by the Hong Kong RGC 16302223.
文摘We propose a simple embedding method for computing the eigenvalues and eigenfunctions of the Laplace-Beltrami operator on implicit surfaces.The approach follows an embedding approach for solving the surface eikonal equation.We replace the differential operator on the interface with a typical Cartesian differential operator in the surface neighborhood.Our proposed algorithm is easy to implement and efficient.We will give some two-and three-dimensional numerical examples to demonstrate the effectiveness of our proposed approach.
基金funding from the National Natural Science Foundation of China(no.51872173)Natural Science Foundation of Shandong Province(no.ZR2022JQ21)+2 种基金Higher School Youth Innovation Team of Shandong Province(no.2019KJA013)Hong Kong Scholars Program(no.XJ2019042)Innovationand Technology Commission of the Hong Kong Special Administrative Region(no.ITC-CNERC14EG03)
文摘At present,the research on highly active and stable nitrogen reduction reaction catalysts is still challenging work for the electrosynthesis of ammonia(NH_(3)).Herein,we synthesized atomically dispersed zinc active sites supported on N-doped carbon nanosheets(Zn/NC NSs)as an efficient nitrogen reduction reaction catalyst,which achieves a high ammonia yield of 46.62μg h^(-1)mg^(-1)_(cat).at-0.85 V(vs RHE)and Faradaic efficiency of 95.8%at-0.70 V(vs RHE).In addition,Zn/NC NSs present great stability and selectivity,and there is no significant change in NH_(3)rate and Faradaic efficiencies after multiple cycles.The structural characterization shows that the active center in the nitrogen reduction reaction process is the Zn-N_(4)sites in the catalyst.DFT calculation confirms that Zn/NC with Zn-N_(4)configuration has a lower energy barrier for the formation of^(*)NNH intermediate compared with pure N-doped carbon nanosheets(N-C NSs),thus promoting the hydrogenation kinetics in the whole nitrogen reduction reaction process.
基金supported by the grants from the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.C5031-20)the Guangdong Major Project of Basic and Applied Basic Research(2023B0303000002).
文摘Zinc metal anodes are gaining popularity in aqueous electrochemical energy storage systems for their high safety,cost-effectiveness,and high capacity.However,the service life of zinc metal anodes is severely constrained by critical challenges,including dendrites,water-induced hydrogen evolution,and passivation.In this study,a protective two-dimensional metal–organic framework interphase is in situ constructed on the zinc anode surface with a novel gel vapor deposition method.The ultrathin interphase layer(~1μm)is made of layer-stacking 2D nanosheets with angstrom-level pores of around 2.1Å,which serves as an ion sieve to reject large solvent–ion pairs while homogenizes the transport of partially desolvated zinc ions,contributing to a uniform and highly reversible zinc deposition.With the shielding of the interphase layer,an ultra-stable zinc plating/stripping is achieved in symmetric cells with cycling over 1000 h at 0.5 mA cm−2 and~700 h at 1 mA cm^(−2),far exceeding that of the bare zinc anodes(250 and 70 h).Furthermore,as a proof-of-concept demonstration,the full cell paired with MnO_(2) cathode demonstrates improved rate performances and stable cycling(1200 cycles at 1 A g−1).This work provides fresh insights into interphase design to promote the performance of zinc metal anodes.
基金financial support from the Guangzhou Municipal Government.
文摘Lithium metal batteries(LMBs)are considered the ideal choice for high volumetric energy density lithium-ion batteries,but uncontrolled lithium deposition poses a significant challenge to the stability of such devices.In this paper,we introduce a 2.5μm-thick asymmetric and ultrastrong separator,which can induce tissue-like lithium deposits.The asymmetric separator,denoted by utPE@Cu_(2)O,was prepared by selective synthesis of Cu_(2)O nanoparticles on one of the outer surfaces of a nanofibrous(diameter~10 nm)ultrastrong ultrahigh molecular weight polyethylene(UHMWPE)membrane.Microscopic analysis shows that the lithium deposits have tissue-like morphology,resulting in the symmetric lithium cells assembled using utPE@Cu_(2)O with symmetric Cu_(2)O coating exhibiting stable performance for over 2000 h of cycling.This work demonstrates the feasibility of a facile approach ultrathin separators for the deployment of lithium metal batteries,providing a pathway towards enhanced battery performance and safety.
基金supported by the General Program of Chongqing Natural Science Foundation(CSTB2022NSCQMSX1227 and CSTB2022NSCQ-MSX0459)the supports from the Fundamental Research Funds for the Central Universities(SWU-XDJH202314)。
文摘Although the performance of perovskite solar cells(PSCs)has been dramatically increased in recent years,stability is still the main obstacle preventing the PSCs from being commercial.PSC device instability can be caused by a variety of reasons,including ions diffusion,surface and grain boundary defects,etc.In this work,the cross-linkable tannic acid(TA)is introduced to modify perovskite film through post-treatment method.The numerous organic functional groups(–OH and C=O)in TA can interact with the uncoordinated Pb^(2+)and I^(-)ions in perovskite,thus passivating defects and inhibiting ions diffusion.In addition,the formed TA network can absorb a small amount of the residual moisture inside the device to protect the perovskite layer.Furthermore,TA modification regulates the energy level of perovskite,and reduces interfacial charge recombination.Ultimately,following TA treatment,the device efficiency is increased significantly from 21.31%to 23.11%,with a decreased hysteresis effect.Notably,the treated device shows excellent air,thermal,and operational stability.In light of this,the readily available,inexpensive TA has the potential to operate as a multipurpose interfacial modifier to increase device efficiency while also enhancing device stability.
基金R.Ma thanks the support from PolyU Distinguished Postdoc Fellowship(1-YW4C)Z.Luo thanks the National Natural Science Foundation of China(NSFC,No.22309119)+7 种基金J.Wu thanks the Guangdong government and the Guangzhou government for funding(2021QN02C110)the Guangzhou Municipal Science and Technology Project(No.2023A03J0097 and 2023A03J0003)H.Yan appreciates the support from the National Key Research and Development Program of China(No.2019YFA0705900)funded by MOST,the Basic and Applied Research Major Program of Guangdong Province(No.2019B030302007)the Shen Zhen Technology and Innovation Commission through(Shenzhen Fundamental Research Program,JCYJ20200109140801751)the Hong Kong Research Grants Council(research fellow scheme RFS2021-6S05,RIF project R6021-18,CRF project C6023‐19G,GRF project 16310019,16310020,16309221,and 16309822)Hong Kong Innovation and Technology Commission(ITC‐CNERC14SC01)Foshan‐HKUST(Project NO.FSUST19‐CAT0202)Zhongshan Municipal Bureau of Science and Technology(NO.ZSST20SC02)and Tencent Xplorer Prize。
文摘With plenty of popular and effective ternary organic solar cells(OSCs)construction strategies proposed and applied,its power conversion efficiencies(PCEs)have come to a new level of over 19%in single-junction devices.However,previous studies are heavily based in chloroform(CF)leaving behind substantial knowledge deficiencies in understanding the influence of solvent choice when introducing a third component.Herein,we present a case where a newly designed asymmetric small molecular acceptor using fluoro-methoxylated end-group modification strategy,named BTP-BO-3FO with enlarged bandgap,brings different morphological evolution and performance improvement effect on host system PM6:BTP-eC9,processed by CF and ortho-xylene(o-XY).With detailed analyses supported by a series of experiments,the best PCE of 19.24%for green solvent-processed OSCs is found to be a fruit of finely tuned crystalline ordering and general aggregation motif,which furthermore nourishes a favorable charge generation and recombination behavior.Likewise,over 19%PCE can be achieved by replacing spin-coating with blade coating for active layer deposition.This work focuses on understanding the commonly met yet frequently ignored issues when building ternary blends to demonstrate cutting-edge device performance,hence,will be instructive to other ternary OSC works in the future.
基金supported by is supported by the Shanghai Municipal Science and Technology Major Projectthe support from Shanghai Super Postdoctoral Incentive Program
文摘Focusing on revealing the origin of high ammonia yield rate on Cu via nitrate reduction(NO3RR),we herein applied constant potential method via grand-canonical density functional theory(GC-DFT)with implicit continuum solvation model to predict the reaction energetics of NO3RR on pure copper surface in alkaline media.The potential-dependent mechanism on the most prevailing Cu(111)and the minor(100)and(110)facets were established,in consideration of NO_(2)_(−),NO,NH_(3),NH_(2)OH,N_(2),and N_(2)O as the main products.The computational results show that the major Cu(111)is the ideal surface to produce ammonia with the highest onset potential at 0.06 V(until−0.37 V)and the highest optimal potential at−0.31 V for ammonia production without kinetic obstacles in activation energies at critical steps.For other minor facets,the secondary Cu(100)shows activity to ammonia from−0.03 to−0.54 V with the ideal potential at−0.50 V,which requires larger overpotential to overcome kinetic activation energy barriers.The least Cu(110)possesses the longest potential range for ammonia yield from−0.27 to−1.12 V due to the higher adsorption coverage of nitrate,but also with higher tendency to generate di-nitrogen species.Experimental evaluations on commercial Cu/C electrocatalyst validated the accuracy of our proposed mechanism.The most influential(111)surface with highest percentage in electrocatalyst determined the trend of ammonia production.In specific,the onset potential of ammonia production at 0.1 V and emergence of yield rate peak at−0.3 V in experiments precisely located in the predicted potentials on Cu(111).Four critical factors for the high ammonia yield and selectivity on Cu surface via NO3RR are summarized,including high NO3RR activity towards ammonia on the dominant Cu(111)facet,more possibilities to produce ammonia along different pathways on each facet,excellent ability for HER inhibition and suitable surface size to suppress di-nitrogen species formation at high nitrate coverage.Overall,our work provides comprehensive potential-dependent insights into the reaction details of NO3RR to ammonia,which can serve as references for the future development of NO3RR electrocatalysts,achieving higher activity and selectivity by maximizing these characteristics of copper-based materials.
基金funded by the Hong Kong Research Grants Council(25201620/C6001-22Y)the Hong Kong Innovation Technology Commission(ITC)under project No.MHP/060/21support of the State Key Laboratory of Advanced Displays and Optoelectronics Technologies at HKUST.
文摘Electronic waste(e-waste)and diabetes are global challenges to modern societies.However,solving these two challenges together has been challenging until now.Herein,we propose a laser-induced transfer method to fabricate portable glucose sensors by recycling copper from e-waste.We bring up a laser-induced full-automatic fabrication method for synthesizing continuous heterogeneous Cu_(x)O(h-Cu_(x)O)nano-skeletons electrode for glucose sensing,offering rapid(<1 min),clean,air-compatible,and continuous fabrication,applicable to a wide range of Cu-containing substrates.Leveraging this approach,h-Cu_(x)O nanoskeletons,with an inner core predominantly composed of Cu_(2)O with lower oxygen content,juxtaposed with an outer layer rich in amorphous Cu_(x)O(a-Cu_(x)O)with higher oxygen content,are derived from discarded printed circuit boards.When employed in glucose detection,the h-Cu_(x)O nano-skeletons undergo a structural evolution process,transitioning into rigid Cu_(2)O@CuO nano-skeletons prompted by electrochemical activation.This transformation yields exceptional glucose-sensing performance(sensitivity:9.893 mA mM^(-1) cm^(-2);detection limit:0.34μM),outperforming most previously reported glucose sensors.Density functional theory analysis elucidates that the heterogeneous structure facilitates gluconolactone desorption.This glucose detection device has also been downsized to optimize its scalability and portability for convenient integration into people’s everyday lives.
基金supported by the Research Grants Council,University Grants Committee,Hong Kong SAR(Project Number:N_PolyU552/20)supported by the National Nature Science Foundation of China(22209138)Guangdong Basic and Applied Basic Research Foundation(2021A1515110464).
文摘Reversible protonic ceramic cells(RePCCs)hold promise for efficient energy storage,but their practicality is hindered by a lack of high-performance air electrode materials.Ruddlesden-Popper perovskite Sr_(3)Fe_(2)O_(7−δ)(SF)exhibits superior proton uptake and rapid ionic conduction,boosting activity.However,excessive proton uptake during RePCC operation degrades SF’s crystal structure,impacting durability.This study introduces a novel A/B-sites co-substitution strategy for modifying air electrodes,incorporating Sr-deficiency and Nb-substitution to create Sr_(2.8)Fe_(1.8)Nb_(0.2)O_(7−δ)(D-SFN).Nb stabilizes SF’s crystal,curbing excessive phase formation,and Sr-deficiency boosts oxygen vacancy concentration,optimizing oxygen transport.The D-SFN electrode demonstrates outstanding activity and durability,achieving a peak power density of 596 mW cm^(−2)in fuel cell mode and a current density of−1.19 A cm^(−2)in electrolysis mode at 1.3 V,650℃,with excellent cycling durability.This approach holds the potential for advancing robust and efficient air electrodes in RePCCs for renewable energy storage.
基金financially supported by the project of the National Natural Science Foundation of China(52202115 and 52172101)the China Postdoctoral Science Foundation(2022M722586)+2 种基金the Natural Science Foundation of Chongqing,China(CSTB2022NSCQ-MSX1085)the Shaanxi Science and Technology Innovation Team(2023-CX-TD-44)the Fundamental Research Funds for the Central Universities(3102019JC005 and G2022KY0604)。
文摘Low-temperature processed electron transport layer(ETL)of TiO_(2)that is widely used in planar perovskite solar cells(PSCs)has inherent low carrier mobility,resulting in insufficient photogenerated elec-tron transport and thus recombination loss at buried interface.Herein,we demonstrate an effective strategy of laser embedding of p-n homojunctions in the TiO_(2)ETL to accelerate electron transport in PSCs,through localized build-in electric fields that enables boosted electron mobility by two orders of magnitude.Such embedding is found significantly helpful for not only the enhanced crystallization quality of TiO_(2)ETL,but the fabrication of perovskite films with larger-grain and the less-trap-states.The embedded p-n homojunction enables also the modulation of interfacial energy level between perovskite layers and ETLs,favoring for the reduced voltage deficit of PSCs.Benefiting from these merits,the formamidinium lead iodide(FAPbI_(3))PSCs employing such ETLs deliver a champion efficiency of 25.50%,along with much-improved device stability under harsh conditions,i.e.,maintain over 95%of their initial efficiency after operation at maximum power point under continuous heat and illumination for 500 h,as well as mixed-cation PSCs with a champion efficiency of 22.02%and over 3000 h of ambient storage under humidity stability of 40%.Present study offers new possibilities of regulating charge transport layers via p-n homojunction embedding for high performance optoelectronics.
基金supported by the Research Grants Council(26206115,16304821 and 16309418)the Southern Marine Science and Engineering Guangdong Laboratory(Guangzhou)(SMSEGL20SC01)+2 种基金the Innovation and Technology Commission(grant no.ITC-CNERC14EG03)of the Hong Kong Special Administrative Regionthe Hong Kong Postdoctoral Fellowship Scheme(HKUST PDFS2021-4S12 and HKUST PDFS2021-6S08)the support from the Shenzhen fundamental research funding(JCYJ20210324115809026,20200925154115001,JCYJ20200109141216566)。
文摘Urea generation through electrochemical CO_(2) and NO_(3)~-co-reduction reaction(CO_(2)NO_(3)RR)is still limited by either the low selectivity or yield rate of urea.Herein,we report copper carbonate hydroxide(Cu_2(OH)_2CO_(3))as an efficient CO_(2)NO_(3)RR electrocatalyst with an impressive urea Faradaic efficiency of45.2%±2.1%and a high yield rate of 1564.5±145.2μg h~(-1)mg_(cat)~(-1).More importantly,H_(2) evolution is fully inhibited on this electrocatalyst over a wide potential range between-0.3 and-0.8 V versus reversible hydrogen electrode.Our thermodynamic simulation reveals that the first C-N coupling follows a unique pathway on Cu_2(OH)_2CO_(3) by combining the two intermediates,~*COOH and~*NHO.This work demonstrates that high selectivity and yield rate of urea can be simultaneously achieved on simple Cu-based electrocatalysts in CO_(2)NO_(3)RR,and provide guidance for rational design of more advanced catalysts.
基金supported by the National Key Research and Development Program of China(Grant Nos.2021YFB3800100 and 2021YFB3800101)the National Natural Science Foundation of China(62004089,U2001217,and U19A2089)+6 种基金the Guangdong Basic and Applied Basic Research Foundation(2019A1515110439,2019B1515120083,and2022A1515011218)the Shenzhen Science and Technology Program(JCYJ20190809150811504 and KQTD2015033110182370)the HKRGC General Research Funds(16312216)the Shenzhen&Hong Kong Joint Research Program(SGLH20180622092406130)the Shenzhen Engineering Research and Development Center for Flexible Solar Cel s Project funding from Shenzhen Development and Reform Committee(2019-126)the Key Fundamental Research Project funding from the Shenzhen Science and Technology Innovation Committee(JCYJ20200109141014474)the Guangdong-Hong Kong-Macao Joint Laboratory(2019B121205001)
文摘Hole transport material free carbon-based all-inorganic CsPbBr_(3)perovskite solar cells(PSCs)are promising for commercialization due to its low-cost,high open-circuit voltage(V_(oc))and superior stability.Due to the different solubility of PbBr_(2)and CsBr in conventional solvents,CsPbBr_(3)films are mainly obtained by multi-step spin-coating through the phase evolution from PbBr_(2)to CsPb_(2)Br_(5)and then to CsPbBr_(3).The scalable fabrication of high-quality CsPbBr_(3)films has been rarely studied.Herein,an inkjet-printing method is developed to prepare high-quality CsPbBr_(3)films.The formation of long-range crystalline CsPb_(2)Br_(5)phase can effectively improve phase purity and promote regular crystal stacking of CsPbBr_(3).Consequently,the inkjet-printed CsPbBr_(3)C-PSCs realized PCEs up to 9.09%,8.59%and 7.81%with active areas of 0.09,0.25,and 1 cm^(2),respectively,demonstrating the upscaling potential of our fabrication method and devices.This high performance is mainly ascribed to the high purity,strong crystal orientation,reduced surface roughness and lower trap states density of the as-printed CsPbBr_(3)films.This work provides insights into the relationship between the phase evolution mechanisms and crystal growth dynamics of cesium lead bromide halide films.
基金financially supported by the General Research Fund(16309918)from the Research Grant Council,Hong Kongfunding from the Institute for Advanced Study of the Hong Kong University of Science and Technology。
文摘Close-space sublimation(CSS)has been demonstrated as an alternative vacuum deposition technique for fabricating organic light-emitting diodes(OLEDs).CSS utilizes a planar donor plate pre-coated with organic thin films as an area source to rapidly transfer the donor film to a device substrate at temperatures below 200℃.CSS is also conformal and capable of depositing on odd-shaped substrates using flexible donor media.The evaporation behaviors of organic donor films under CSS were fully characterized using model OLED materials and CSS-deposited films exhibited comparable device performances in an OLED stack to films deposited by conventional point sources.The low temperature and conformal nature of CSS,along with its high material utilization and short process time,make it a promising method for fabricating flexible OLED displays.
基金supported by the National Natural Science Foundation of China(No.22074025)Guangzhou Municipal Science and Technology Project(No.202102010473)+5 种基金Science and Technology Program of Guangdong Province(2019B090905007)National Science Foundation of Guangdong Province(2021A1515010078)the Scientific and Technological Plan of Guangdong Province(2019B090905007)Natural Science Foundation of Shandong Province(Grant No.ZR2023QE059)China Postdoctoral Science Foundation(Grant No.2021M700915)Guangdong Basic and Applied Basic Research Foundation(2020A1515111086,2020A1515110219,and 2020A1515110770)for the financial support.
文摘Tailoring the interfacial interaction in SiCbased anode materials is crucial to the accomplishment of higher energy capacities and longer cycle lives for lithium-ion storage.In this paper,atomic-scale tunable interfacial interaction is achieved by epitaxial growth of high-quality N doped graphene(NG)on SiC(NG@SiC).This well-designed NG@SiC heterojunction demonstrates an intrinsic electric field with intensive interfacial interaction,making it an ideal prototype to thoroughly understand the configurations of electron/ion bridges and the mechanisms of interatomic electron migration.Both density functional theory(DFT)analysis and electrochemical kinetic analysis reveal that these intriguing electron/ion bridges can control and tailor the interfacial interaction via the interfacial coupled chemical bonds,enhancing the interfacial charge transfer kinetics and preventing pulverization/aggregation.As a proof-of-concept study,this well-designed NG@SiC anode shows good reversible capacity(1197.5 mAh g^(−1)after 200 cycles at 0.1 A g^(−1))and cycling durability with 76.6%capacity retention at 447.8 mAh g^(−1)after 1000 cycles at 10.0 A g^(−1).As expected,the lithium-ion full cell(LiFePO_(4)/C//NG@SiC)shows superior rate capability and cycling stability.This interfacial interaction tailoring strategy via epitaxial growth method provides new opportunities for traditional SiC-based anodes to achieve high-performance lithium-ion storage and beyond.
基金supported by the Science and Technology Plan of Shenzhen(JCYJ20170818114107730,JCYJ20180306174923335)The General Research Fund(projects 16205321,16214619)from the Hong Kong Research Grant Council,Innovation Technology Fund(GHP/014/19SZ)+2 种基金Guangdong-Hong Kong-Macao Intelligent Micro-Nano Optoelectronic Technology Joint Laboratory(2020B1212030010)Foshan Innovative and Entrepreneurial Research Team Program(2018IT100031)the support from the Center for 1D/2D Quantum Materials and the State Key Laboratory of Advanced Displays and Optoelectronics Technologies at HKUST。
文摘The high-density,vertically aligned retinal neuron array provides effective vision,a feature we aim to replicate with electronic devices.However,the conventional complementary metal-oxide-semiconductor(CMOS)image sensor,based on separate designs for sensing,memory,and processing units,limits its integration density.Moreover,redundant signal communication significantly increases energy consumption.Current neuromorphic devices integrating sensing and signal processing show promise in various computer vision applications,but there is still a need for frame-based imaging with good compatibility.In this study,we developed a dual-mode image sensor based on a high-density all-inorganic perovskite nanowire array.The device can switch between frame-based standard imaging mode and neuromorphic imaging mode by applying different biases.This unique bias-dependent photo response is based on a well-designed energy band diagram.The biomimetic alignment of nanowires ensures the potential for high-resolution imaging.To further demonstrate the imaging ability,we conducted pattern reconstruction in both modes with a 10×10 crossbar device.This study introduces a novel image sensor with high compatibility and efficiency,suitable for various applications including computer vision,surveillance,and robotics.
文摘Organic-inorganic halides perovskites(OHPs)have drawn the attention of many researchers owing to their astonishing and unique optoelectronic properties.They have been extensively used for photovoltaic applications,achieving higher than 26%power conversion efficiency to date.These materials have potential to be deployed for many other applications beyond photovoltaics like photodetectors,sensors,light-emitting diodes(LEDs),and resistors.To address the looming challenge of Moore’s law and the Von Neumann bottleneck,many new technologies regarding the computation of architectures and storage of information are being extensively researched.Since the discovery of the memristor as a fourth component of the circuit,many materials are explored for memristive applications.Lately,researchers have advanced the exploration of OHPs for memristive applications.These materials possess promising memristive properties and various kinds of halide perovskites have been used for different applications that are not only limited to data storage but expand towards artificial synapses,and neuromorphic computing.Herein we summarize the recent advancements of OHPs for memristive applications,their unique electronic properties,fabrication of materials,and current progress in this field with some future perspectives and outlooks.
基金supported by the Department of Science and Technology of Guangdong Province(2019A050510043)。
文摘Rechargeable aprotic Li-O_(2)batteries have attractea increasing attention due to their extremely high capacity,and it is very important to design appropriate strategies to synthesize efficient catalysts used as oxygen cathode.In present work,we present an expedient "instantaneous nucleation and epitaxial growth"(INEG) synthesis strategy for convenient and large-scale synthesis of ultrafine MOCPs nanoparticles(size 50-100 nm) with obvious advantages such as fast synthesis,high yields,low costs and reduced synthetic steps.The bimetallic Ru/Co-MOCPs are further pyrolyzed to obtain bimetallic Coand low content of Ru-based nanoparticles embedded within nitrogen-doped carbon(Ru/Co@N-C) as an efficient catalyst used in Li-O_(2)battery.The Ru/Co@N-C provides porous carbon framework for the ion transportation and O_(2)diffusion,and has large amounts of metal/nonmetal sites as active site to promote the oxygen reduction reaction(ORR)/oxygen evolution reaction(OER) in Li-O_(2)batteries.As a consequence,a high discharge specific capacity of 15246 mA h g^(-1)at 250 mA g^(-1), excellent rate capability at different current densities,and stable overpotential during cycling,are achieved.This work opened up a new understanding for the industrialized synthesis of ultrafine catalysts for Li-O_(2)batteries with excellent structural characteristics and electrochemical performance.
基金Project(51964033) supported by the National Natural Science Foundation of ChinaProject supported by the Youth Talent in Ten Thousand Talents Plan of Yunnan Province,ChinaProject supported by the Scientist Studio of Yunnan Province,China。
基金fundings from the National Natural Science Foundation of China (No. 51872173)Taishan Scholar Foundation of Shandong Province (No. tsqn201812068)+3 种基金Natural Science Foundation of Shandong Province (No. ZR2022JQ21)Higher School Youth Innovation Team of Shandong Province (No. 2019KJA013)Hong Kong Scholars Program (No. XJ2019042)Innovation and Technology Commission of the Hong Kong Special Administrative Region (No. ITC-CNERC14EG03)。
文摘Hydrophobic treatment of the catalyst surfaces can suppress the competitive hydrogen evolution reaction(HER) during the nitrogen reduction reaction(NRR).In this work,the surface of Ti_(3)C_(2)Ti_(x) MXene is modified by cetyltrimethylammonium bromide(CTAB) and trimethoxy(3,3,4,4,5,5,6,6,7,7,8,8,8-trideca fluorooctyl) silane(FOTS) to increase the hydrophobicity of MXenes.The ammonia(NH_(3)) production rate and faradaic efficiency(FE) are improved from 37.62 to 54.01 μg h^(-1)mg_(cat)^(-1).and 5.5% to 18.1% at-0.7 V vs.RHE,respectively after surface modification.^(15)N isotopic labeling experiment confirms that nitrogen in produced ammonia originates from N_(2) in the electrolyte.The excellent NRR activity of surface hydrophobic MXenes is mainly due to surfactant molecules,which inhibit the entry of water molecules and the competitive HER,which have been verified by in situ FT-IR,DFT and molecular dynamics calculations.This strategy provides an ingenious method to design more active NRR electrocatalysts.