In recent years,renewable energy sources,which aim to replace rapidly depleting fossil fuels,face challenges due to limited energy storage and conversion technologies.To enhance energy storage and conversion efficienc...In recent years,renewable energy sources,which aim to replace rapidly depleting fossil fuels,face challenges due to limited energy storage and conversion technologies.To enhance energy storage and conversion efficiency,extensive research has been conducted in the academic community on numerous potential materials.Among these materials,metal fluorides have attracted significant attention due to their ionic metal-fluorine bonds and tunable electronic structures,attributed to the highest electronegativity of fluorine in their chemical composition.This makes them promising candidates for future electrochemical applications in various fields.However,metal fluorides encounter various challenges in different application directions.Therefore,we comprehensively review the applications of metal fluorides in the field of energy storage and conversion,aiming to deepen our understanding of their exhibited characteristics in different electrochemical processes.In this paper,we summarize the difficulties and improvement methods encountered in different types of battery applications and several typical electrode optimization strategies in the field of supercapacitors.In the field of water electrolysis,we focus on surface reconstruction and the critical role of fluorine,demonstrating the catalytic performance of metal fluorides from the perspectives of reconstruction mechanism and process analysis.Finally,we provide a summary and outlook for this field,aiming to offer guidance for future breakthroughs in the energy storage and conversion applications of metal fluorides.展开更多
Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indiu...Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indium tin oxide(ITO)surface and the desorption of hydroxyl(OH)from the ITO surface induced by polar solvents can lead to the formation of vacancies.Herein,a dimethylacridine-based SAM is incorporated into the perovskite precursor solution.This SAM can be extruded from the precursor solution and enriched on the bottom surface of the perovskite,filling the vacancies and in situ forming a mixed SAM with MeO-2PACz as a hole-selective layer(HSL).The in situ formed mixed SAM optimizes the energy level alignment between the HSL and the perovskite,facilitating hole extraction and alleviating the residual strain of the perovskite film.Consequently,the perovskite solar cells(PSCs),based on the mixed SAM,achieve a power conversion efficiency(PCE)of 25.69%and exhibit excellent operational stability.When this approach is applied to 1.78 eV bandgap PSC devices,it yields a PCE of 20.08%.This work presents a unique strategy for fabricating both high-quality perovskite films and superior buried interfaces,which is also applicable to wide-bandgap PSCs.展开更多
Two-dimensional(2D)heterostructures compris-ing of differently stacking atomic layers are attrac-tive owing to its flexible composition as well as the emerging new physicochemical properties.Howev-er,so far many 2D ve...Two-dimensional(2D)heterostructures compris-ing of differently stacking atomic layers are attrac-tive owing to its flexible composition as well as the emerging new physicochemical properties.Howev-er,so far many 2D vertical heterojunctions are constructed through transfer methods,inevitably introducing interfacial impurities and thus hindering detailed atomic-level studies.In this work,we have developed a clean two-step fabrication strat-egy by combining ultrahigh vacuum(UHV)molecular beam epitaxy(MBE)growth with am-bient chemical vapor deposition(CVD).We first-ly grew single crystalline graphene film on a SiC substrate under UHV condition,and then synthesized MoS_(2)films on the graphene-SiC sur-face through CVD under inert atmosphere,thus successfully realized the construction of a well-defined MoS_(2)-graphene/SiC heterojunction with clean surface.Particularly,we observed the MoS_(2)can not only grow into monolayer flakes but also form spiral structures,the latter showing layer-by-layer stacks with reduced bandgap down to~1.0 eV.展开更多
Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimat...Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.展开更多
Isolated cationic Pd species encapsulated in MFI zeolite,i.e.,Pd@MFI,have been successfully prepared via in situ hydrothermal route followed by oxidative treatment.The as-prepared Pd@MFI samples are investigated as pr...Isolated cationic Pd species encapsulated in MFI zeolite,i.e.,Pd@MFI,have been successfully prepared via in situ hydrothermal route followed by oxidative treatment.The as-prepared Pd@MFI samples are investigated as promising catalysts in the reaction of methane combustion.Typically,Pd@H-ZSM-5 shows remarkable activity in methane catalytic combustion with a low apparent activation energy value of 70.7 kj/mol as well as good catalytic stability even in excess water vapor.Detailed characterization results demonstrate the strong interaction between Pd sites and zeolite framework in Pd@ZSM-5 and the efficient stabilization of isolated Pd sites by zeolite thereof.Spectroscopy analyses reveal that the presence of BrΦnsted acid sites is beneficial to methane adsorption and its subsequent activation on adjacent Pd sites,constructing cooperation between Bronsted acid sites and Pd sites within the confined space of MFI zeolite toward high-efficiency methane catalytic combustion.The reaction mechanism of methane combustion catalyzed by Pd@H-ZSM-5 model catalyst is finally discussed.展开更多
Propane dehydrogenation(PDH), employing Pt-or Cr-based catalysts, represents an emerging industrial route for propylene production. Due to the scarcity of platinum and the toxicity of chromium, alternative PDH catalys...Propane dehydrogenation(PDH), employing Pt-or Cr-based catalysts, represents an emerging industrial route for propylene production. Due to the scarcity of platinum and the toxicity of chromium, alternative PDH catalysts are being pursued. Herein, we report the construction of Zn-containing zeolite catalysts,namely Zn@S-1, for PDH reaction. Well-isolated zinc cations are successfully trapped and stabilized by the Si-OH groups in S-1 zeolites via in-situ hydrothermal synthesis. The as-prepared Zn@S-1 catalysts exhibit good dehydrogenation activity, high propylene selectivity, and regeneration capability in PDH reaction under employed conditions. The in-situ partial reduction of zinc species is observed and the partially reduced zinc cations are definitely identified as the active sites for PDH reaction.展开更多
The inhomogeneous broadening parameter and the internal loss of green LDs are determined by experiments and theoretical fitting. It is found that the inhomogeneous broadening plays an important role on the threshold c...The inhomogeneous broadening parameter and the internal loss of green LDs are determined by experiments and theoretical fitting. It is found that the inhomogeneous broadening plays an important role on the threshold current density of green LDs. The green LD with large inhomogeneous broadening even cannot lase. Therefore, reducing inhomogeneous broadening is a key issue to improve the performance of green LDs.展开更多
Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discove...Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discover that the current collector can dramatically affect the performance of flexible electrochemical power sources with large size. For flexible air-breathing proton exchange membrane fuel cell (PEMFC), the performance could have more than 8 times increase by only adjusting the directions of current collectors. The different performances of different current collection types are mainly attributed to the diverse lengths of the electron transfer pathways. In addition, the conductivity of current collector can dramatically affect the capability of flexible PEMFCs with large-size. The flexible PEMFCs with thicker carbon nanotube membrane as current collector (low electric resistance) show higher ability. A mathematic model is successfully built in this work to further understand the performance. Moreover, the model and simulation are also applicable to other flexible power sources, such as flexible Li-ion battery and supercapacitor.展开更多
Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft h...Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(<5μm)hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.展开更多
High quality gallium oxide(Ga_2O_3) thin films are deposited by remote plasma-enhanced atomic layer deposition(RPEALD) with trimethylgallium(TMG) and oxygen plasma as precursors. By introducing in-situ NH3 plasma pret...High quality gallium oxide(Ga_2O_3) thin films are deposited by remote plasma-enhanced atomic layer deposition(RPEALD) with trimethylgallium(TMG) and oxygen plasma as precursors. By introducing in-situ NH3 plasma pretreatment on the substrates, the deposition rate of Ga_2O_3 films on Si and GaN are remarkably enhanced, reached to 0.53 and 0.46 ?/cycle at 250 °C,respectively. The increasing of deposition rate is attributed to more hydroxyls(–OH) generated on the substrate surfaces after NH3 pretreatment, which has no effect on the stoichiometry and surface morphology of the oxide films, but only modifies the surface states of substrates by enhancing reactive site density. Ga_2O_3 film deposited on GaN wafer is crystallized at 250 °C, with an epitaxial interface between Ga_2O_3 and GaN clearly observed. This is potentially very important for reducing the interface state density through high quality passivation.展开更多
Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoret...Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoretical and experimental works have been devoted to exploring various possibilities to increase the functionality and the specific capacitance of electrodes for SCs. Non-carbon two-dimensional(2D)materials have been considered as encouraging electrode candidates for their chemical and physical advantages such as tunable surface chemistry, high electronic conductivity, large mechanical strength, more active sites, and dual non-faradaic and faradaic electrochemical performances. Besides, these 2D materials also play particular roles in constructing highway channels for fast ion diffusion. This concise review summarizes cutting-edge progress of some representative 2D non-carbon materials for the aqueous electrolyte-based SCs, including transition metal oxides(TMOs), transition metal hydroxides(TMHs), transition metal chalcogenides(TMCs), MXenes, metal-organic frameworks(MOFs) and some emerging materials. Different synthetic methods, effective structural designs and corresponding electrochemical performances are reviewed in detail. And we finally present a detailed discussion of the current intractable challenges and technical bottlenecks, and highlight future directions and opportunities for the development of next-generation high-performance energy storage devices.展开更多
Lithium metal is regarded as the ultimate negative electrode material for secondary batteries due to its high energy density.However,it suffers from poor cycling stability because of its high reactivity with liquid el...Lithium metal is regarded as the ultimate negative electrode material for secondary batteries due to its high energy density.However,it suffers from poor cycling stability because of its high reactivity with liquid electrolytes.Therefore,continuous efforts have been put into improving the cycling Coulombic efficiency(CE)to extend the lifespan of the lithium metal negative electrode.Herein,we report that using dual-salt additives of LiPF_(6) and LiNO_(3) in an ether solvent-based electrolyte can significantly improve the cycling stability and rate capability of a Li-carbon(Li-CNT)composite.As a result,an average cycling CE as high as 99.30% was obtained for the Li-CNT at a current density of 2.5 mA cm^(-2) and an negative electrode to positive electrode capacity(N/P)ratio of 2.The cycling stability and rate capability enhancement of the Li-CNT negative electrode could be attributed to the formation of a better solid electrolyte interphase layer that contains both inorganic components and organic polyether.The former component mainly originates from the decomposition of the LiNO_(3) additive,while the latter comes from the LiPF_(6)-induced ring-opening polymerization of the ether solvent.This novel surface chemistry significantly improves the CE of Li negative electrode,revealing its importance for the practical application of lithium metal batteries.展开更多
Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C couplin...Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.展开更多
Electrocatalytic reduction of carbon dioxide is one of the most effective strategies to achieve carbon neutrality and energy sustainability.Although high-value multi-carbon products have been widely studied,limited el...Electrocatalytic reduction of carbon dioxide is one of the most effective strategies to achieve carbon neutrality and energy sustainability.Although high-value multi-carbon products have been widely studied,limited electrocatalysts have been reported for the selective conversion of ethane.More importantly,the factors tuning the selectivity between ethane and ethylene have not been clarified.Here,Zn@Cu nanowire arrays(Zn@Cu-NWAs) catalyst is proposed to stimulate the maintenance of efficient CO_(2)-to-C_(2)H_(6) conversion at high current densities.Meanwhile,in order to investigate the factors affecting the interconversion between ethane and ethylene,the counterpart catalyst that facilitates C–C coupling to ethylene was also synthesized.Time-of-flight secondary-ion mass spectroscopy(TOF-SIMS),in-situ Raman spectroscopy,and simulation results show that Zn@Cu-NWAs can provide a localized proton corridor environment for the formation of ethane,accelerating the further proton-coupled CO_(2) reduction reaction(CO_(2)RR)kinetics.Hence,this catalyst delivered an ethane Faraday efficiency of over 65% at-1.14 V vs.RHE with a total current density of 142.3 mA/cm^(2).This work provides a new perspective on regulating the local microenvironment to modify the selectivity of multi-carbon products.展开更多
Infrared(IR)absorption spectroscopy has been widely used for dynamic characterization of catalysts and mechanism of catalytic reactions.However,due to the strong infrared absorption of heterogeneous catalysts(mainly o...Infrared(IR)absorption spectroscopy has been widely used for dynamic characterization of catalysts and mechanism of catalytic reactions.However,due to the strong infrared absorption of heterogeneous catalysts(mainly oxides,or supported metal and metal oxides,etc.)below 1200 cm^(-1),and the intensity of regular infrared light source rapidly decays at low-wavenumber range,most in-situ infrared spectroscopy studies are limited to the detection of surface adsorbates in the range of 4000-900 cm^(-1).The change of catalytically active component itself(M-O,M-M bond,etc.,1200-50 cm^(-1))during the reaction is hard to be tracked under reaction conditions by in-situ IR.In this work,a home-made in-situ IR reactor was designed and a sample preparing method was developed.With such progresses,the changes of reactants,products,surface adsorbates,and catalysts themselves can be measured under the same reaction conditions with a spectral range of 4000-400 cm^(-1),providing a new opportunity for in-situ characterization of heterogeneous catalysis.CO oxidation on Pd/SiO_(2) and Cu/SiO_(2) catalysts were taken as examples,since both the two catalytic systems were extensively used commercially,and moreover reduction and oxidation of palladium and copper occur during the examined reaction conditions.The characteristic bands of Pd^(2+)-O(670,608 cm^(-1)),Cu^(+)-O(635 cm^(-1))and Cu^(2+)-O(595,535 cm^(-1))were observed by IR,and the changes during CO oxidation reaction were successfully monitored by IR.The oxidation/reduction of palladium and copper were also confirmed by ex-situ XPS.Moreover,Pd^(0) in Pd/SiO_(2) and Cu^(+)in Cu/SiO_(2) were found as the thermal dynamically stable phases under the examined conditions for CO oxidation.展开更多
Graphene,as a saturable absorber(SA),has attracted much attention for its application in ultrashort pulse fiber lasers due to its ultrafast interband carrier relaxation and ultra-broadband wavelength operation.Neverth...Graphene,as a saturable absorber(SA),has attracted much attention for its application in ultrashort pulse fiber lasers due to its ultrafast interband carrier relaxation and ultra-broadband wavelength operation.Nevertheless,during the stacking process of monolayer graphene layer,the induced nonuniform contact at the interface of graphene layers deteriorate the device performance.Herein,we report the fabrication of graphene saturable absorber mirrors(SAMs)via a one-step transfer process and the realization of the much enlarged modulation depth and the much reduced nonsaturable loss with tri-layer graphene(TLG)than single-layer graphene(SLG)due to the improved uniform contact at the interface.Moreover,the operation of 1550 nm mode-locked Er-doped fiber laser with the TLG SAM exhibits excellent output characteristics of the maximum output power of 9.9 mW,a slope efficiency of 2.4%and a pulse width of 714 fs.Our findings are expected to pave the way toward high-performance ultrashort pulse fiber lasers based on graphene SAs.展开更多
Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage p...Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage performance of SCs.However,none of the conventional electrolytes can fully meet the increasing requirements of SCs in terms of high ion conductivity,excellent stability,wide voltage window and operating temperature range,as well as environmentally friend concerns.To this end,hybrid electrolytes have sprung up in recent years,which are believed to be the candidate to solve these shortcomings.Herein,the state-of-the-art types of hybrid electrolytes for SCs,including the combination of aqueous and organic,aqueous and gel polymer,ionic liquids(ILs)and organic,and ILs and gel polymer hybrid electrolytes,are reviewed.The effects of different hybrid systems on the performance of SCs and the underlying mechanisms are among the focal points of the review,and prospects and possible directions are discussed as well to provide further insight into the future development of this field.展开更多
GaInP alloy could be the most trusted key material for fabricating super-high-efficiency single-and multijunction solar cells, especially for space applications. The storage and transfer of optical excitation energy i...GaInP alloy could be the most trusted key material for fabricating super-high-efficiency single-and multijunction solar cells, especially for space applications. The storage and transfer of optical excitation energy in this key alloy is thus a key subject of the energy conversion from optical to electrical. In this article we present a study of the subject through investigating photoluminescence(PL) degradation in the GaInP epilayer at 4 K under the continuous optical excitations of ultraviolet(UV) 325 nm, visible 488.0 and 514.5 nm lasers. It is found that the decline of PL intensity with the irradiation time may be represented by I(t)/I0=(1 + tτ-1)-1+C, where I0 is the luminescence intensity at the beginning of irradiation, a time constant, and C a background. Moreover, the PL degradation degree reduces with increasing the excitation wavelength. In addition, some red shift of the PL peak is observed accompanying with the intensity decline under the UV laser excitation. These PL signatures indicate that the localized carriers within the local atomic ordering domains play a major role in the storage and transfer of the excitation energy via photon recycling processes.展开更多
As a special order of electronic correlation induced by spatial modulation, the charge density wave(CDW) phenomena in condensed matters attract enormous research interests. Here, using scanning-tunneling microscopy in...As a special order of electronic correlation induced by spatial modulation, the charge density wave(CDW) phenomena in condensed matters attract enormous research interests. Here, using scanning-tunneling microscopy in various temperatures, we discover a hidden incommensurate stripe-like CDW order besides the(■) CDW phase at low-temperature of 4 K in the epitaxial monolayer 1T-VSe_(2) film. Combining the variable-temperature angle-resolved photoemission spectroscopic(ARPES) measurements, we discover a two-step transition of an anisotropic CDW gap structure that consists of two parts △_(1) and△_(2). The gap part ?1 that closes around ~ 150 K is accompanied with the vanish of the(√7×√3) CDW phase. While another momentum-dependent gap part △_(2) can survive up to ~ 340 K, and is suggested to the result of the incommensurate CDW phase. This two-step transition with anisotropic gap opening and the resulted evolution in ARPES spectra are corroborated by our theoretical calculation based on a phenomenological form for the self-energy containing a two-gap structure △_(1) +△_(2), which suggests different forming mechanisms between the(√7×√3) and the incommensurate CDW phases. Our findings provide significant information and deep understandings on the CDW phases in monolayer 1T-VSe_(2) film as a two-dimensional(2D) material.展开更多
Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from...Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from two-dimensional planar to three-dimensional nanoparticles were prepared by atomic layer deposition(ALD) method. By combing scanning tunneling microscopy(STM) and X-ray photoelectron spectroscopy(XPS) at near-ambient pressure of CO_(2) hydrogenation, we reveal that the submonolayer ZnO/Cu(111) transformed into Cu-Zn alloy under 10 mbar CO_(2)/H_(2) at 493 K, and underwent a partial reoxidation during evacuation. The dynamic phase transformation of ZnO/Cu(111) may partly explain the existence of differences and apparently contradictory theories to account for the origin of active phase in CZA catalysts.展开更多
基金National Natural Science Foundation of China,Grant/Award Number:51073067Scientific and Technological Development Program of Jilin Province,Grant/Award Number:20220201138GX.
文摘In recent years,renewable energy sources,which aim to replace rapidly depleting fossil fuels,face challenges due to limited energy storage and conversion technologies.To enhance energy storage and conversion efficiency,extensive research has been conducted in the academic community on numerous potential materials.Among these materials,metal fluorides have attracted significant attention due to their ionic metal-fluorine bonds and tunable electronic structures,attributed to the highest electronegativity of fluorine in their chemical composition.This makes them promising candidates for future electrochemical applications in various fields.However,metal fluorides encounter various challenges in different application directions.Therefore,we comprehensively review the applications of metal fluorides in the field of energy storage and conversion,aiming to deepen our understanding of their exhibited characteristics in different electrochemical processes.In this paper,we summarize the difficulties and improvement methods encountered in different types of battery applications and several typical electrode optimization strategies in the field of supercapacitors.In the field of water electrolysis,we focus on surface reconstruction and the critical role of fluorine,demonstrating the catalytic performance of metal fluorides from the perspectives of reconstruction mechanism and process analysis.Finally,we provide a summary and outlook for this field,aiming to offer guidance for future breakthroughs in the energy storage and conversion applications of metal fluorides.
基金supported by the Young Cross Team Project of CAS(No.JCTD-2021-14)the National Natural Science Foundation of China(51925206)Gusu Innovation and Entrepreneur Leading Talents(ZXL2022466)。
文摘Self-assembled monolayers(SAMs),owing to their amphiphilic nature,tend to aggregate,which impedes the formation of a dense and uniform SAM on the substrate.Additionally,the weak adsorption ability of SAMs on the indium tin oxide(ITO)surface and the desorption of hydroxyl(OH)from the ITO surface induced by polar solvents can lead to the formation of vacancies.Herein,a dimethylacridine-based SAM is incorporated into the perovskite precursor solution.This SAM can be extruded from the precursor solution and enriched on the bottom surface of the perovskite,filling the vacancies and in situ forming a mixed SAM with MeO-2PACz as a hole-selective layer(HSL).The in situ formed mixed SAM optimizes the energy level alignment between the HSL and the perovskite,facilitating hole extraction and alleviating the residual strain of the perovskite film.Consequently,the perovskite solar cells(PSCs),based on the mixed SAM,achieve a power conversion efficiency(PCE)of 25.69%and exhibit excellent operational stability.When this approach is applied to 1.78 eV bandgap PSC devices,it yields a PCE of 20.08%.This work presents a unique strategy for fabricating both high-quality perovskite films and superior buried interfaces,which is also applicable to wide-bandgap PSCs.
基金support from the Natural Science Foundation of Jiangsu Province(No.BK20210124)the National Natural Science Foun-dation of China(No.12204512,No.22172152,No.21872130,No.22372193)+3 种基金the National Key Re-search and Development Program of China(No.2021YFA1502801)the joint funds from the Hefei National Synchrotron Radiation Laboratory(No.KY2060000202)We also acknowledge financial support from the CAS Project for Young Scientists in Basic Research(No.YSBR-049)the Fundamental Re-search Funds for the Central Universities(No.WK3510000013,WK2060000066).
文摘Two-dimensional(2D)heterostructures compris-ing of differently stacking atomic layers are attrac-tive owing to its flexible composition as well as the emerging new physicochemical properties.Howev-er,so far many 2D vertical heterojunctions are constructed through transfer methods,inevitably introducing interfacial impurities and thus hindering detailed atomic-level studies.In this work,we have developed a clean two-step fabrication strat-egy by combining ultrahigh vacuum(UHV)molecular beam epitaxy(MBE)growth with am-bient chemical vapor deposition(CVD).We first-ly grew single crystalline graphene film on a SiC substrate under UHV condition,and then synthesized MoS_(2)films on the graphene-SiC sur-face through CVD under inert atmosphere,thus successfully realized the construction of a well-defined MoS_(2)-graphene/SiC heterojunction with clean surface.Particularly,we observed the MoS_(2)can not only grow into monolayer flakes but also form spiral structures,the latter showing layer-by-layer stacks with reduced bandgap down to~1.0 eV.
基金supported by the Natural Science Foundation of China(22309179)the Natural Science Foundation of China(12404049)+4 种基金Natural Science Foundation of Ningxia(2023AAC01003)Guangdong Basic and Applied Basic Research Foundation(2021A1515110156,2022A1515010724,2023A1515110521,2023B1515120095,2024A1515011260)Science and Technology Program of Guangzhou(No.2019050001)the Outstanding Youth Project of Guangdong Natural Science Foundation(2021B1515020051)Dalian Revitalization Talents Program(No.2022RG01).
文摘Developing electrocatalysts to inhibit polysulfide shuttling and expedite sulfur species conversion is vital for the evolution of Lithium-sulfur(Li-S)batteries.This work provides a facile strategy to design an intimate heterostructure of MIL-88A@CdS as a sulfur electrocatalyst combining high sulfur adsorption and accelerated polysulfide conversion.The MIL-88A can give a region of high-ordered polysulfide adsorption,whereas the CdS is an effective nanoreactor for the sulfur reduction reaction(SRR).Notedly,the significant size difference between MIL-88A and CdS enables the unique heterostructure interactions.The largesize MIL-88A ensures a uniform distribution of CdS nanoparticles as a substrate.This configuration facilitates control of the initial polysulfide adsorption position relative to its final deposition site as lithium sulfide.The heterostructure also demonstrates rapid transport and efficient conversion of lithium polysulfides.Consequently,the Li-S battery with MIL-88A@CdS heterostructure modified separator delivers exceptional performance,achieving an areal capacity exceeding 6 mAh cm^(−2),an excellent rate capability of 980 mAh g^(−1) at 5 C,and notable cycling stability in a 2 Ah pouch cell over 100 cycles.This work is significant for elucidating the relationship between heterostructure and electrocatalytic performance,providing great insights for material design aimed at highly efficient future electrocatalysts in practical applications.
文摘Isolated cationic Pd species encapsulated in MFI zeolite,i.e.,Pd@MFI,have been successfully prepared via in situ hydrothermal route followed by oxidative treatment.The as-prepared Pd@MFI samples are investigated as promising catalysts in the reaction of methane combustion.Typically,Pd@H-ZSM-5 shows remarkable activity in methane catalytic combustion with a low apparent activation energy value of 70.7 kj/mol as well as good catalytic stability even in excess water vapor.Detailed characterization results demonstrate the strong interaction between Pd sites and zeolite framework in Pd@ZSM-5 and the efficient stabilization of isolated Pd sites by zeolite thereof.Spectroscopy analyses reveal that the presence of BrΦnsted acid sites is beneficial to methane adsorption and its subsequent activation on adjacent Pd sites,constructing cooperation between Bronsted acid sites and Pd sites within the confined space of MFI zeolite toward high-efficiency methane catalytic combustion.The reaction mechanism of methane combustion catalyzed by Pd@H-ZSM-5 model catalyst is finally discussed.
基金National Natural Science Fund of China(22025203, 21872072)the Municipal Natural Science Fund of Tianjin (18JCJQJC47400) for supporting the work。
文摘Propane dehydrogenation(PDH), employing Pt-or Cr-based catalysts, represents an emerging industrial route for propylene production. Due to the scarcity of platinum and the toxicity of chromium, alternative PDH catalysts are being pursued. Herein, we report the construction of Zn-containing zeolite catalysts,namely Zn@S-1, for PDH reaction. Well-isolated zinc cations are successfully trapped and stabilized by the Si-OH groups in S-1 zeolites via in-situ hydrothermal synthesis. The as-prepared Zn@S-1 catalysts exhibit good dehydrogenation activity, high propylene selectivity, and regeneration capability in PDH reaction under employed conditions. The in-situ partial reduction of zinc species is observed and the partially reduced zinc cations are definitely identified as the active sites for PDH reaction.
基金supported by the National Key Research and Development Program of China(Grant Nos.2017YFB0405000,2016YFB0401803)the National Natural Science Foundation of China(Grant Nos.61834008,61574160,and 61704184)support of the Chinese Academy of Science Visiting Professorship for Senior International Scientists (Grant No.2013T2J0048)
文摘The inhomogeneous broadening parameter and the internal loss of green LDs are determined by experiments and theoretical fitting. It is found that the inhomogeneous broadening plays an important role on the threshold current density of green LDs. The green LD with large inhomogeneous broadening even cannot lase. Therefore, reducing inhomogeneous broadening is a key issue to improve the performance of green LDs.
基金financial support granted by Ministry of Science and Technology of China(Nos. 2016YFE0105700, 2016YFA0200700)the National Natural Science Foundation of China (Nos. 21373264, 21573275)+2 种基金China Postdoctoral Science Foundation(No. 2018M632406)the Science and Technology Project of Nanchang(No. 2017-SJSYS-008)the Collaborative Innovation Center of Suzhou Nano Science and Technology
文摘Flexible electrochemical power sources are attracting increasing attentions for their unique advantages like flexibility, shape diversity, light weight and excellent mechanical properties. In this research, we discover that the current collector can dramatically affect the performance of flexible electrochemical power sources with large size. For flexible air-breathing proton exchange membrane fuel cell (PEMFC), the performance could have more than 8 times increase by only adjusting the directions of current collectors. The different performances of different current collection types are mainly attributed to the diverse lengths of the electron transfer pathways. In addition, the conductivity of current collector can dramatically affect the capability of flexible PEMFCs with large-size. The flexible PEMFCs with thicker carbon nanotube membrane as current collector (low electric resistance) show higher ability. A mathematic model is successfully built in this work to further understand the performance. Moreover, the model and simulation are also applicable to other flexible power sources, such as flexible Li-ion battery and supercapacitor.
基金the funding support from the fellowship of the China Postdoctoral Science Foundation (2022M722329, 2021M700097)the National Natural Science Foundation for Distinguished Young Scholars of China (62125112)+2 种基金the National Natural Science Foundation of China (62071462, 62071463, 62271479, 22109173)the Jiangxi Provincial Natural Science Foundation (20224ACB212001)the support from Nano-X Vacuum Interconnected Workstation&Key Laboratory of Multifunctional Nanomaterials and Smart Systems of Suzhou Institute of Nano-Tech and Nano-Bionics (SINANO),Chinese Academy of Sciences (CAS)
文摘Hydrogels offer tissue-like softness,stretchability,fracture toughness,ionic conductivity,and compatibility with biological tissues,which make them promising candidates for fabricating flexible bioelectronics.A soft hydrogel film offers an ideal interface to directly bridge thin-film electronics with the soft tissues.However,it remains difficult to fabricate a soft hydrogel film with an ultrathin configuration and excellent mechanical strength.Here we report a biological tissue-inspired ultrasoft microfiber composite ultrathin(<5μm)hydrogel film,which is currently the thinnest hydrogel film as far as we know.The embedded microfibers endow the composite hydrogel with prominent mechanical strength(tensile stress~6 MPa)and anti-tearing property.Moreover,our microfiber composite hydrogel offers the capability of tunable mechanical properties in a broad range,allowing for matching the modulus of most biological tissues and organs.The incorporation of glycerol and salt ions imparts the microfiber composite hydrogel with high ionic conductivity and prominent anti-dehydration behavior.Such microfiber composite hydrogels are promising for constructing attaching-type flexible bioelectronics to monitor biosignals.
基金supported jointly by the National Natural Science Foundation of China(Nos.61674165,61604167,61574160,61704183,61404159,11604366)the Natural Science Foundation of Jiangsu Province(Nos.BK20170432,BK20160397,BK20140394)+2 种基金the National Key R&D Program of China(No.2016YFB0401803)the Strategic Priority Re-search Program of the Chinese Academy of Science(No.XDA09020401)the support at the Platform for Characterization&Test,Suzhou Institute of Nano-Tech and Nano-Bionics(SINANO),Chinese Academy of Sciences
文摘High quality gallium oxide(Ga_2O_3) thin films are deposited by remote plasma-enhanced atomic layer deposition(RPEALD) with trimethylgallium(TMG) and oxygen plasma as precursors. By introducing in-situ NH3 plasma pretreatment on the substrates, the deposition rate of Ga_2O_3 films on Si and GaN are remarkably enhanced, reached to 0.53 and 0.46 ?/cycle at 250 °C,respectively. The increasing of deposition rate is attributed to more hydroxyls(–OH) generated on the substrate surfaces after NH3 pretreatment, which has no effect on the stoichiometry and surface morphology of the oxide films, but only modifies the surface states of substrates by enhancing reactive site density. Ga_2O_3 film deposited on GaN wafer is crystallized at 250 °C, with an epitaxial interface between Ga_2O_3 and GaN clearly observed. This is potentially very important for reducing the interface state density through high quality passivation.
基金financial support from National Natural Science Foundation of China (No. 21671173)the Independent Designing Scientific Research Project of Zhejiang Normal University (No. 2020ZS03)Zhejiang Provincial Ten Thousand Talent Program (No. 2017R52043)。
文摘Supercapacitors(SCs) with high power density and long cycling span life are demanding energy storage devices that will be an attractive power solution to modern electronic and electrical applications. Numerous theoretical and experimental works have been devoted to exploring various possibilities to increase the functionality and the specific capacitance of electrodes for SCs. Non-carbon two-dimensional(2D)materials have been considered as encouraging electrode candidates for their chemical and physical advantages such as tunable surface chemistry, high electronic conductivity, large mechanical strength, more active sites, and dual non-faradaic and faradaic electrochemical performances. Besides, these 2D materials also play particular roles in constructing highway channels for fast ion diffusion. This concise review summarizes cutting-edge progress of some representative 2D non-carbon materials for the aqueous electrolyte-based SCs, including transition metal oxides(TMOs), transition metal hydroxides(TMHs), transition metal chalcogenides(TMCs), MXenes, metal-organic frameworks(MOFs) and some emerging materials. Different synthetic methods, effective structural designs and corresponding electrochemical performances are reviewed in detail. And we finally present a detailed discussion of the current intractable challenges and technical bottlenecks, and highlight future directions and opportunities for the development of next-generation high-performance energy storage devices.
基金the National Natural Science Foundation of China(Grant nos.21625304 and 21733012)the Ministry of Science and Technology(Grant No.2016YFA0200703).
文摘Lithium metal is regarded as the ultimate negative electrode material for secondary batteries due to its high energy density.However,it suffers from poor cycling stability because of its high reactivity with liquid electrolytes.Therefore,continuous efforts have been put into improving the cycling Coulombic efficiency(CE)to extend the lifespan of the lithium metal negative electrode.Herein,we report that using dual-salt additives of LiPF_(6) and LiNO_(3) in an ether solvent-based electrolyte can significantly improve the cycling stability and rate capability of a Li-carbon(Li-CNT)composite.As a result,an average cycling CE as high as 99.30% was obtained for the Li-CNT at a current density of 2.5 mA cm^(-2) and an negative electrode to positive electrode capacity(N/P)ratio of 2.The cycling stability and rate capability enhancement of the Li-CNT negative electrode could be attributed to the formation of a better solid electrolyte interphase layer that contains both inorganic components and organic polyether.The former component mainly originates from the decomposition of the LiNO_(3) additive,while the latter comes from the LiPF_(6)-induced ring-opening polymerization of the ether solvent.This novel surface chemistry significantly improves the CE of Li negative electrode,revealing its importance for the practical application of lithium metal batteries.
基金financial support from the National Key R&D Program of China (Nos. 2022YFA1504500, 2022YFA1503100)the National Natural Science Foundation of China (Nos. 21988101, 21890753, 22225204, 92145301, 22002160 and 22272174)+4 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences (No. XDB36030200)the CAS Project for Young Scientists in Basic Research (No. YSBR-028)the Fundamental Research Funds for the Central Universities (No. 20720220008)the Dalian National Lab for Clean Energy (DNL Cooperation Fund 202001)the Innovation Research Fund Project of DICP (No. DICP I202016)。
文摘Electrochemical CO reduction reaction(CORR) provides a promising approach for producing valuable multicarbon products(C_(2+)), while the low solubility of CO in aqueous solution and high energy barrier of C–C coupling as well as the competing hydrogen evolution reaction(HER) largely limit the efficiency for C_(2+)production in CORR. Here we report an overturn on the Faradaic efficiency of CORR from being HER-dominant to C_(2+)formation-dominant over a wide potential window, accompanied by a significant activity enhancement over a Moss-like Cu catalyst via pressuring CO. With the CO pressure rising from 1 to 40 atm, the C_(2+)Faradaic efficiency and partial current density remarkably increase from 22.8%and 18.9 mA cm^(-2)to 89.7% and 116.7 mA cm^(-2), respectively. Experimental and theoretical investigations reveal that high pressure-induced high CO coverage on metallic Cu surface weakens the Cu–C bond via reducing electron transfer from Cu to adsorbed CO and restrains hydrogen adsorption, which significantly facilitates the C–C coupling while suppressing HER on the predominant Cu(111) surface, thereby boosting the CO electroreduction to C_(2+)activity.
基金financially supported by the Outstanding Youth Project of Guangdong Natural Science Foundation (2021B1515020051)the financial support from the Basic and Applied Basic Research Foundation of Guangdong Province (2021B1515120024, 2022A1515011804)。
文摘Electrocatalytic reduction of carbon dioxide is one of the most effective strategies to achieve carbon neutrality and energy sustainability.Although high-value multi-carbon products have been widely studied,limited electrocatalysts have been reported for the selective conversion of ethane.More importantly,the factors tuning the selectivity between ethane and ethylene have not been clarified.Here,Zn@Cu nanowire arrays(Zn@Cu-NWAs) catalyst is proposed to stimulate the maintenance of efficient CO_(2)-to-C_(2)H_(6) conversion at high current densities.Meanwhile,in order to investigate the factors affecting the interconversion between ethane and ethylene,the counterpart catalyst that facilitates C–C coupling to ethylene was also synthesized.Time-of-flight secondary-ion mass spectroscopy(TOF-SIMS),in-situ Raman spectroscopy,and simulation results show that Zn@Cu-NWAs can provide a localized proton corridor environment for the formation of ethane,accelerating the further proton-coupled CO_(2) reduction reaction(CO_(2)RR)kinetics.Hence,this catalyst delivered an ethane Faraday efficiency of over 65% at-1.14 V vs.RHE with a total current density of 142.3 mA/cm^(2).This work provides a new perspective on regulating the local microenvironment to modify the selectivity of multi-carbon products.
文摘Infrared(IR)absorption spectroscopy has been widely used for dynamic characterization of catalysts and mechanism of catalytic reactions.However,due to the strong infrared absorption of heterogeneous catalysts(mainly oxides,or supported metal and metal oxides,etc.)below 1200 cm^(-1),and the intensity of regular infrared light source rapidly decays at low-wavenumber range,most in-situ infrared spectroscopy studies are limited to the detection of surface adsorbates in the range of 4000-900 cm^(-1).The change of catalytically active component itself(M-O,M-M bond,etc.,1200-50 cm^(-1))during the reaction is hard to be tracked under reaction conditions by in-situ IR.In this work,a home-made in-situ IR reactor was designed and a sample preparing method was developed.With such progresses,the changes of reactants,products,surface adsorbates,and catalysts themselves can be measured under the same reaction conditions with a spectral range of 4000-400 cm^(-1),providing a new opportunity for in-situ characterization of heterogeneous catalysis.CO oxidation on Pd/SiO_(2) and Cu/SiO_(2) catalysts were taken as examples,since both the two catalytic systems were extensively used commercially,and moreover reduction and oxidation of palladium and copper occur during the examined reaction conditions.The characteristic bands of Pd^(2+)-O(670,608 cm^(-1)),Cu^(+)-O(635 cm^(-1))and Cu^(2+)-O(595,535 cm^(-1))were observed by IR,and the changes during CO oxidation reaction were successfully monitored by IR.The oxidation/reduction of palladium and copper were also confirmed by ex-situ XPS.Moreover,Pd^(0) in Pd/SiO_(2) and Cu^(+)in Cu/SiO_(2) were found as the thermal dynamically stable phases under the examined conditions for CO oxidation.
基金supported by the Key Research and Development Plan of Ministry of Science and Technology(2016YFB0402303)National Natural Science Foundation of China(NSFC)(61875222,61605106)China Postdoctoral Science Foundation(2017M621858)
文摘Graphene,as a saturable absorber(SA),has attracted much attention for its application in ultrashort pulse fiber lasers due to its ultrafast interband carrier relaxation and ultra-broadband wavelength operation.Nevertheless,during the stacking process of monolayer graphene layer,the induced nonuniform contact at the interface of graphene layers deteriorate the device performance.Herein,we report the fabrication of graphene saturable absorber mirrors(SAMs)via a one-step transfer process and the realization of the much enlarged modulation depth and the much reduced nonsaturable loss with tri-layer graphene(TLG)than single-layer graphene(SLG)due to the improved uniform contact at the interface.Moreover,the operation of 1550 nm mode-locked Er-doped fiber laser with the TLG SAM exhibits excellent output characteristics of the maximum output power of 9.9 mW,a slope efficiency of 2.4%and a pulse width of 714 fs.Our findings are expected to pave the way toward high-performance ultrashort pulse fiber lasers based on graphene SAs.
基金financial support from the National Natural Science Foundation of China(21671173)Zhejiang Provincial Ten Thousand Talent Program(2017R52043)。
文摘Supercapacitors(SCs)are emerging as efficient energy storage devices but still suffering from limited energy density compared with batteries.Electrolytes have been regarded as the key to determine the energy storage performance of SCs.However,none of the conventional electrolytes can fully meet the increasing requirements of SCs in terms of high ion conductivity,excellent stability,wide voltage window and operating temperature range,as well as environmentally friend concerns.To this end,hybrid electrolytes have sprung up in recent years,which are believed to be the candidate to solve these shortcomings.Herein,the state-of-the-art types of hybrid electrolytes for SCs,including the combination of aqueous and organic,aqueous and gel polymer,ionic liquids(ILs)and organic,and ILs and gel polymer hybrid electrolytes,are reviewed.The effects of different hybrid systems on the performance of SCs and the underlying mechanisms are among the focal points of the review,and prospects and possible directions are discussed as well to provide further insight into the future development of this field.
基金supported by the National Natural Science Foundation of China (Grant No. 11374247)in part by a grant from the University Grants Committee Areas of Excellence Scheme of the Hong Kong Special Administrative Region, China (Project No. [AoE/P-03/08])
文摘GaInP alloy could be the most trusted key material for fabricating super-high-efficiency single-and multijunction solar cells, especially for space applications. The storage and transfer of optical excitation energy in this key alloy is thus a key subject of the energy conversion from optical to electrical. In this article we present a study of the subject through investigating photoluminescence(PL) degradation in the GaInP epilayer at 4 K under the continuous optical excitations of ultraviolet(UV) 325 nm, visible 488.0 and 514.5 nm lasers. It is found that the decline of PL intensity with the irradiation time may be represented by I(t)/I0=(1 + tτ-1)-1+C, where I0 is the luminescence intensity at the beginning of irradiation, a time constant, and C a background. Moreover, the PL degradation degree reduces with increasing the excitation wavelength. In addition, some red shift of the PL peak is observed accompanying with the intensity decline under the UV laser excitation. These PL signatures indicate that the localized carriers within the local atomic ordering domains play a major role in the storage and transfer of the excitation energy via photon recycling processes.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 92165205, 11790311, 12004172, 11774152, 11604366, and 11634007)the National Key Research and Development Program of China (Grant Nos. 2018YFA0306800 and 2016YFA0300401)+1 种基金the Program of High-Level Entrepreneurial and Innovative Talents Introduction of Jiangsu Province, the Jiangsu Planned Projects for Postdoctoral Research Funds (Grant No. 2020Z172)the Natural Science Foundation of Jiangsu Province, China (Grant No. BK 20160397)。
文摘As a special order of electronic correlation induced by spatial modulation, the charge density wave(CDW) phenomena in condensed matters attract enormous research interests. Here, using scanning-tunneling microscopy in various temperatures, we discover a hidden incommensurate stripe-like CDW order besides the(■) CDW phase at low-temperature of 4 K in the epitaxial monolayer 1T-VSe_(2) film. Combining the variable-temperature angle-resolved photoemission spectroscopic(ARPES) measurements, we discover a two-step transition of an anisotropic CDW gap structure that consists of two parts △_(1) and△_(2). The gap part ?1 that closes around ~ 150 K is accompanied with the vanish of the(√7×√3) CDW phase. While another momentum-dependent gap part △_(2) can survive up to ~ 340 K, and is suggested to the result of the incommensurate CDW phase. This two-step transition with anisotropic gap opening and the resulted evolution in ARPES spectra are corroborated by our theoretical calculation based on a phenomenological form for the self-energy containing a two-gap structure △_(1) +△_(2), which suggests different forming mechanisms between the(√7×√3) and the incommensurate CDW phases. Our findings provide significant information and deep understandings on the CDW phases in monolayer 1T-VSe_(2) film as a two-dimensional(2D) material.
基金financially supported by the National Natural Science Foundation of China (No. 91845109, No. 21872169)。
文摘Sustainable methanol production via CO_(2) hydrogenation leads to increased interest in the understanding of active phase of Cu/ZnO/Al_(2)O_(3)(CZA) catalyst. Model catalysts of ZnO/Cu(111) with structures varied from two-dimensional planar to three-dimensional nanoparticles were prepared by atomic layer deposition(ALD) method. By combing scanning tunneling microscopy(STM) and X-ray photoelectron spectroscopy(XPS) at near-ambient pressure of CO_(2) hydrogenation, we reveal that the submonolayer ZnO/Cu(111) transformed into Cu-Zn alloy under 10 mbar CO_(2)/H_(2) at 493 K, and underwent a partial reoxidation during evacuation. The dynamic phase transformation of ZnO/Cu(111) may partly explain the existence of differences and apparently contradictory theories to account for the origin of active phase in CZA catalysts.
