查看更多>>摘要：Developing suitable photocatalysts and understanding their intrinsic catalytic mechanism remain key challenges in the pursuit of highly active,good selective,and long-term stable photocatalytic CO2 reduc-tion(PCO2R)systems.Herein,monoclinic Cu2(OH)2CO3 is firstly proven to be a new class of photocatalyst,which has excellent catalytic stability and selectivity for PCO2R in the absence of any sacrificial agent and cocatalysts.Based on a Cu2(OH)23CO3 photocatalyst and 13CO2 two-sided 13C isotopic tracer strategy,and combined with in situ diffused reflectance infrared Fourier transform spectroscopy(DRIFTS)analysis and density functional theory(DFT)calculations,two main CO2 transformation routes,and the photo-decomposition and self-restructuring dynamic equilibrium mechanism of Cu2(OH)2CO3 are definitely revealed.The PCO2R activity of Cu2(OH)2CO3 is comparable to some of state-of-the-art novel photocata-lysts.Significantly,the PCO2R properties can be further greatly enhanced by simply combining Cu2(OH)2CO3 with typical TiO2 to construct composites photocatalyst.The highest CO and CH4 production rates by 7.5 wt％Cu2(OH)2CO3-TiO2 reach 16.4 μmol g-1h-1 and 116.0 μmol g-1h1,respectively,which are even higher than that of some of PCO2R systems containing sacrificial agents or precious metals mod-ified photocatalysts.This work provides a better understanding for the PCO2R mechanism at the atomic levels,and also indicates that basic carbonate photocatalysts have broad application potential in the future.
查看更多>>摘要：Over the years,zinc-ion batteries(ZIBs)have attracted attention as a promising next-generation energy storage technology because of their excellent safety,long cycling performance,eco-friendliness,and high-power density.However,issues,such as the corrosion and dissolution of the Zn anode,limited wet-tability,and lack of sufficient nucleation sites for Zn plating,have limited their practical application.The introduction of a protective layer comprising of tellurium(Te)nanobelts onto the surface of Zn anode has emerged as a promising approach to overcome these limitations and improve the electrochemical behav-ior by enhancing the safety and wettability of ZIBs,as well as providing numerous nucleation sites for Zn plating.In the presence of a Te-based protective layer,the energy power density of the surface-engineered Zn anode improved significantly(ranging from 310 to 144 W h kg-1,over a power density range of 270 to 1,800 W kg-1),and the lifespan capability was extended.These results demonstrate that the proposed strategy of employing Te nanobelts as a protective layer holds great promise for enhancing the energy storage performance of ZIBs,making them even more attractive as a viable energy storage solution for the future.
查看更多>>摘要：The interfaces between the inorganic metal oxide and organic photoactive layer are of outmost impor-tance for efficiency and stability in organic solar cells(OSCs).Tin oxide(SnO2)is one of the promising can-didates for the electron transport layer(ETL)in high-performance inverted OSCs.When a solution-processed SnO2 ETL is employed,however,the presence of interfacial defects and suboptimal interfacial contact can lower the power conversion efficiency(PCE)and operational stability of OSCs.Herein,highly efficient and stable inverted OSCs by modification of the SnO2 surface with ultraviolet(UV)-curable acry-late oligomers(SAR and OCS)are demonstrated.The highest PCEs of 16.6％and 17.0％are achieved in PM6:Y6-BO OSCs with the SAR and OCS,respectively,outperforming a device with a bare SnO2 ETL(PCE 13.8％).The remarkable enhancement of PCEs is attributed to the optimized interfacial contact,leading to miti-gated surface defects.More strikingly,improved light-soaking and thermal stability strongly correlated with the interfacial defects are demonstrated for OSCs based on SnO2/UV cross-linked resins compared to OSCs utilizing bare SnO2.We believe that UV cross-linking oligomers will play a key role as interfacial modifiers in the future fabrication of large-area and flexible OSCs with high efficiency and stability.
查看更多>>摘要：The absence of control over carriers transport during electrochemical cycling,accompanied by the dete-rioration of the solid electrolyte interphase(SEI)and the growth of lithium dendrites,has hindered the development of lithium metal batteries.Herein,a separator complexion consisting of polyacrylonitrile(PAN)nanofiber and MIL-101(Cr)particles prepared by electrospinning is proposed to bind the anions from the electrolyte utilizing abundant effective open metal sites in the MIL-101(Cr)particles to modu-late the transport of non-effective carriers.The binding effect of the PANM separator promotes uniform lithium metal deposition and enhances the stability of the SEI layer and long cycling stability of ultra-high nickel layered oxide cathodes.Taking PANM as the Li||NCM96 separator enables high-voltage cycling stability,maintaining 72％capacity retention after 800 cycles at a charging and discharging rate of 0.2 C at a cut-off voltage of 4.5 V and 0 ℃.Meanwhile,the excellent high-rate performance delivers a specific capacity of 156.3 mA h g-1 at 10 C.In addition,outstanding cycling performance is realized from-20 to 60 ℃.The separator engineering facilitates the electrochemical performance of lithium metal bat-teries and enlightens a facile and promising strategy to develop fast charge/discharge over a wide range of temperatures.
查看更多>>摘要：Surface/interface engineering of a multimetallic nanostructure with diverse electrocatalytic properties for direct liquid fuel cells is desirable yet challenging.Herein,using visible light,a class of quaternary PtAgBiTe ultrathin nanosheets is fabricated and used as high-performance anode electrocatalysts for for-mic acid-/alcohol-air fuel cells.The modified electronic structure of Pt,enhanced hydroxyl adsorption,and abundant exterior defects afford Pt1Ag0.1Bi0.16Te0.29/C high intrinsic anodic electrocatalytic activity to boost the power densities of direct formic acid-/methanol-/ethanol-/ethylene glycol-/glycerol-air fuel cells,and the corresponding peak power density of Pt1Ag0.1Bi0.16Te0.29/C is respectively 129.7,142.3,105.4,124.3,and 128.0 mW cm-2,considerably outperforming Pt/C.Operando in situ Fourier transform infrared reflection spectroscopy reveals that formic acid oxidation on Pt1Ag0.1Bi0.16Te0.29/C occurs via a CO-free direct pathway.Density functional theory calculations show that the presence of Ag,Bi,and Te in Pt1Ag0.1Bi0.16Te0.29 suppresses CO*formation while optimizing dehydrogenation steps and synergis-tic effect and modified Pt effectively enhance H2O dissociation to improve electrocatalytic performance.This synthesis strategy can be extended to 43 other types of ultrathin multimetallic nanosheets(from ternary to octonary nanosheets),and efficiently capture precious metals(i.e.,Pd,Pt,Rh,Ru,Au,and Ag)from different water sources.
查看更多>>摘要：Steering the directional carrier migration across the interface is a central mission for efficient photocat-alytic reactions.In this work,an atomic-shared heterointerface is constructed between the defect-rich ZnIn2S4(HVs-ZIS)and Coln2S4(CIS)via a defect-guided heteroepitaxial growth strategy.The strong inter-face coupling induces adequate carriers exchanging passageway between HVs-ZIS and CIS,enhancing the internal electric field(IEF)in the Znln2S4/CoIn2S4(HVs-ZIS/CIS)heterostructure.The defect structure in HVs-ZIS induces an additional defect level,improving the separation efficiency of photocarriers.Moreover,promoted by the IEF and intimate heterointerface,photogenerated electrons trapped by the defect level can migrate to the valence band of CIS,contributing to massive photogenerated electrons with intense reducibility in HVs-ZIS/CIS.Consequently,the HVs-ZIS/CIS heterostructure performs a boosted H2 evolution activity of 33.65 mmol g-1 h-1.This work highlights the synergistic effects of defect and strong interface coupling in regulating carrier transfer and paves a brave avenue for constructing effi-cient heterostructure photocatalysts.
查看更多>>摘要：Sodium-ion batteries(SIBs)are expected to offer affordability and high energy density for large-scale energy storage system.However,the commercial application of SIBs is hurdled by low initial coulombic efficiency(ICE),continuous Na loss during long-term operation,and low sodium-content of cathode materials.In this scenario,presodiation strategy by introducing an external sodium reservoir has been rationally proposed,which could supplement additional sodium ions into the system and thereby mark-edly improve both the cycling performance and energy density of SIBs.In this review,the significance of presodiation is initially introduced,followed by comprehensive interpretation on technological proper-ties,underlying principles,and associated approaches,as well as our perspectives on present inferiorities and future research directions.Overall,this contribution outlines a distinct pathway towards the preso-diation methodology,of significance but still in its nascent phase,which may inspire the targeted guide-lines to explore new chemistry in this field.
Abdul HananHafiz Taimoor Ahmed AwanFaiza BibiRaja Rafidah Raja Sulaiman...
176-206页
查看更多>>摘要：The increasing focus on electrocatalysis for sustainable hydrogen(H2)production has prompted signifi-cant interest in MXenes,a class of two-dimensional(2D)materials comprising metal carbides,carboni-trides,and nitrides.These materials exhibit intriguing chemical and physical properties,including excellent electrical conductivity and a large surface area,making them attractive candidates for the hydrogen evolution reaction(HER).This scientific review explores recent advancements in MXene-based electrocatalysts for HER kinetics.It discusses various compositions,functionalities,and explicit design principles while providing a comprehensive overview of synthesis methods,exceptional proper-ties,and electro-catalytic approaches for H2 production via electrochemical reactions.Furthermore,chal-lenges and future prospects in designing MXenes-based electrocatalysts with enhanced kinetics are highlighted,emphasizing the potential of incorporating different metals to expand the scope of electro-chemical reactions.This review suggests possible efforts for developing advanced MXenes-based electro-catalysts,particularly for efficient H2 generation through electrochemical water-splitting reactions..
查看更多>>摘要：Metastable nanostructured electrocatalyst with a completely different surface environment compared to conventional phase-based electrocatalyst often shows distinctive catalytic property.Although Ru-based electrocatalysts have been widely investigated toward hydrogen oxidation reaction(HOR)under alkaline electrolytes,these studies are mostly limited to conventional hexagonal-close-packed(hcp)phase,mainly arising from the lack of sufficient synthesis strategies.In this study,we report the precise synthe-sis of metastable binary RuW alloy with face-centered-cubic(fcc)phase.We find that the introduction of W can serve as fcc phase seeds and reduce the formation energy of metastable fcc-RuW alloy.Impressively,fcc-RuW exhibits remarkable alkaline HOR performance and stability with the activity of 0.67 mA cm-2Ru,which is almost five and three times higher than that of hcp-Ru and commercial Pt/C,respectively,which is attributed to the optimized binding strength of adsorbed hydroxide intermediate derived from tailored electronic structure through W doping and phase engineering.Moreover,this strat-egy can also be applied to synthesize other metastable fcc-RuCr and fcc-RuMo alloys with enhanced HOR performances.
查看更多>>摘要：As the primary suppliers of cyclable sodium ions,O3-type layer-structured manganese-based oxides are recognized as highly competitive cathode candidates for sodium-ion batteries.To advance the develop-ment of high-energy sodium-ion batteries,it is crucial to explore cathode materials operating at high voltages while maintaining a stable cycling behavior.The orbital and electronic structure of the octahe-dral center metal element plays a crucial role in maintaining the octahedra structural integrity and improving Na+ion diffusion by introducing heterogeneous chemical bonding.Inspired by the abundant configuration of extra nuclear electrons and large ion radius,we employed trace amounts of tungsten in this study.The obtained cathode material can promote the reversibility of oxygen redox reactions in the high-voltage region and inhibit the loss of lattice oxygen.Additionally,the formation of a Na2WO4 coating on the material surface can improve the interfacial stability and interface ions diffusion.It demonstrates an initial Coulombic efficiency(ICE)of 94.6％along with 168.5 mA h g-1 discharge capacity within the voltage range of 1.9-4.35 V.These findings contribute to the advancement of high-energy sodium-ion batteries by providing insights into the benefits of tungsten doping and Na2WO4 coating on cathode materials.
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