Manar AlnaasanWail Al ZoubiSalh AlhammadiJee-Hyun Kang...
262-273页
查看更多>>摘要：Characterizing and control the chemical compositions of multi-element particles as single metal nanoparticles(mNPs)on the surfaces of catalytic metal oxide supports is challenging.This can be attrib-uted to the heterogeneity and large size at the nanoscale,the poorly defined catalyst nanostructure,and thermodynamic immiscibility of the strongly repelling metallic elements.To address these challenges,an ultrasonic-assisted coincident electro-oxidation-reduction-precipitation(U-SEO-P)is presented to fabri-cate ultra-stable PtRuAgCoCuP NPs,which produces numerous active intermediates and induces strong metal-support interactions.To sort the active high-entropy mNPs,individual NPs are described on the support surface and the role of deep learning in understanding/predicting the features of PtRuAgCoCu@TiOx catalysts is explained.Notably,this deep learning approach required minimal to no human input.The as-prepared PtRuAgCoCu@TiOx catalysts can be used to catalyze various important chemical reactions,such as a high reduction conversion(100％in 30 s),with no loss of catalytic activity even after 20 cycles of nitroarene and ketone/aldehyde,which is several times higher than commercial Pt@TiOx owing to individual PtRuAgCoCuP NPs on TiOx surface.In this study,we present the"Totally Defined Catalysis"concept,which has enormous potential for the advancement of high-activity catalysts in the reduction of organic compounds.
查看更多>>摘要：Lithium-rich manganese-based oxides(LRMOs)exhibit high theoretical energy densities,making them a prominent class of cathode materials for lithium-ion batteries.However,the performance of these lay-ered cathodes often declines because of capacity fading during cycling.This decline is primarily attribu-ted to anisotropic lattice strain and oxygen release from cathode surfaces.Given notable structural transformations,complex redox reactions,and detrimental interface side reactions in LRMOs,the devel-opment of a single modification approach that addresses bulk and surface issues is challenging.Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions.The internal spinel-like phase coating layer,featuring three-dimensional(3D)lithium-ion diffusion channels,effectively blocks oxygen release from the cathode surface and mitigates lattice strain.In addition,the external Li3PO4 coating layer,noted for its superior corrosion resistance,enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals.Notably,the spinel phase,as excellent interlayer,securely anchors Li3PO4 to the bulk lattice and suppresses oxygen release from lattices.Consequently,these modifications considerably boost structural stability and durability,achieving an impressive capacity retention of 83.4％and a minimal voltage decay of 1.49 mV per cycle after 150 cycles at 1 C.These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability.
查看更多>>摘要：The recycling of spent lithium-ion batteries(LIBs)is crucial for environmental protection and resource sustainability.However,the economic recovery of spent LIBs remains challenging due to low Li recovery efficiency and the need for multiple separation operations.Here,we propose a process involving mixed HCl-H2SO4 leaching-spray pyrolysis for recycling spent ternary LIBs,achieving both selective Li recovery and the preparation of a ternary oxide precursor.Specifically,the process transforms spent ternary cath-ode(LiNixCoyMnzO2,NCM)powder into Li2SO4 solution and ternary oxide,which can be directly used for synthesizing battery-grade Li2CO3 and NCM cathode,respectively.Notably,SO42-selectively precipitates with Li+to form thermostable Li2SO4 during the spray pyrolysis,which substantially improves the Li recovery efficiency by inhibiting Li evaporation and intercalation.Besides,SO2 emissions are avoided by controlling the molar ratio of Li+/SO42-(≥2∶1).The mechanism of the preferential formation of Li2SO4 is interpreted from its reverse solubility variation with temperature.During the recycling of spent NCM811,92％of Li is selectively recovered,and the regenerated NCM811 exhibits excellent cycling sta-bility with a capacity retention of 81.7％after 300 cycles at 1 C.This work offers a simple and robust pro-cess for the recycling of spent NCM cathodes.
查看更多>>摘要：Urea is widely used as fertilizer and is a key substance supporting global food production.However,the traditional industrial synthesis of urea faces the challenges with high energy consumption and serious environmental problems.With the increasing global demand for environmental protection and sustain-able development,it is much necessary to develop novel and clean methods for the synthesis of urea.Electrocatalysis provides an efficient and renewable synthesis route that can directly produce urea at room temperature and atmospheric pressure by the coupling of CO2 and nitrogenous molecules.In this review,we summarized the most recent advances in electrochemical synthesis of urea via C-N coupling systematically,focusing on the coupling of CO2 and different nitrogen sources.And the associated cou-pling mechanism,catalysts optimization,and electrolyzer design are well discussed.Moreover,the chal-lenges and future directions for electrocatalytic C—N coupling are prospected.This review will provide timely and valuable guidance for others and attract more interests to promote the development of elec-trochemical synthesis of urea or other valuable chemicals containing C—N bond.
查看更多>>摘要：Zn-based aqueous batteries(ZABs)are gaining widespread popularity due to their low cost and high safety profile.However,the application of ZABs faces significant challenges,such as dendrite growth and parasitic reactions of metallic Zn anodes.Therefore,achieving high-energy-density ZABs necessitates addressing the fundamental thermodynamics and kinetics of Zn anodes.Various strategies are available to mitigate these challenges,with electrolyte additive engineering emerging as one of the most efficient and promising approaches.Despite considerable research in this field,a comprehensive understanding of the intrinsic mechanisms behind the high performance of electrolyte additives remains limited.This review aims to provide a detailed introduction to functional electrolyte additives and thoroughly explore their underlying mechanisms.Additionally,it discusses potential directions and perspectives in additive engineering for ZABs,offering insights into future development and guidelines for achieving high-performance ZABs.
查看更多>>摘要：Rational interface engineering is essential for minimizing interfacial nonradiative recombination losses and enhancing device performance.Herein,we report the use of bidentate diphenoxybenzene(DPOB)isomers as surface modifiers for perovskite films.The DPOB molecules,which contain two oxygen(O)atoms,chemically bond with undercoordinated Pb2+on the surface of perovskite films,resulting in com-pression of the perovskite lattice.This chemical interaction,along with physical regulations,leads to the formation of high-quality perovskite films with compressive strain and fewer defects.This compressive strain-induced band bending promotes hole extraction and transport,while inhibiting charge recombina-tion at the interfaces.Furthermore,the addition of DPOB will reduce the zero-dimensional(0D)Cs4PbBr6 phase and produce the two-dimensional(2D)CsPb2Br5 phase,which is also conducive to the improve-ment of device performance.Ultimately,the resulting perovskite films,which are strain-released and defect-passivated,exhibit exceptional device efficiency,reaching 10.87％for carbon-based CsPbBr3 device,14.86％for carbon-based CsPbI2Br device,22.02％for FA0.97Cs0.03Pbl3 device,respectively.Moreover,the unencapsulated CsPbBr3 PSC exhibits excellent stability under persistent exposure to humidity(80％)and heat(80 ℃)for over 50 days.
查看更多>>摘要：Oxygen reduction reaction(ORR)and oxygen evolution reaction(OER)are the key reactions in numer-ous renewable energy devices.Unlike conventional powdered catalysts,self-supported catalysts are extensively employed in oxygen electrocatalysis because of the enhanced electron-transfer rate,high specific surface area,and superior mechanical flexibility.Among the self-supported conductive sub-strates,carbon fiber usually exhibits several distinctive advantages,such as a straightforward prepara-tion process,relatively low cost,good stability,and excellent conductivity.Against this background,carbon fiber-based self-supported electrocatalysts have been widely applied and studied in oxygen electrocatalysis,indicating a promising development direction in oxygen electrocatalyst research.Thus,it is essential to offer an overall summary of the research progress in this field to facilitate its subsequent development.Taking the regulatory mechanisms and modification methods as a starting point,this review comprehensively summarizes recent research on carbon fiber-based self-supported electrocatalysts in recent years.Firstly,a brief overview of the synthesis methods and regulatory mech-anisms of carbon fiber-based self-supported electrocatalysts is given.Furthermore,the view also high-lights the modification methods and research progress of self-supported electrocatalysts synthesized on carbon fiber-based substrates in recent years in terms of different dopant atoms.Finally,the prospects for the application of self-supported electrocatalysts based on carbon fiber in oxygen electrocatalysis and the possible future directions of their development are presented.This review summarizes recent developments and applications of self-supported bi-functional electrocatalysts with carbon fiber-based materials as the conducting substrate in oxygen electrocatalysis.It also lays a robust scientific founda-tion for the subsequent reasonable design of highly effective carbon fiber-based self-supported electrocatalysts.
查看更多>>摘要：Solar-driven desalination is a promising way to alleviate the freshwater shortage,while is facing chal-lenges posed by low evaporation rates and severe salt accumulation.Herein,a high-performance two-dimensional(2D)solar absorber with Co3O4 nanoneedle arrays(Co3O4-NN)grown on the surface of reduced graphene oxide-coated pyrolyzed silk cloth(Co3O4-NN/rGO/PSC)was prepared,and a salt-free evaporator system was assembled based on the composite material and siphonage-the flowing water delivery.It is revealed that the evaporation enthalpy of water can be reduced over the 2D solar absorber grown with Co3O4-NN,enabling an evaporation rate of up to 2.35 kg m-2 h-1 in DI water under one solar irradiation.The desalination process can be carried out continuously even with salt concentration up to 20 wt％,due to the timely removal of concentrated brine from the interface with the assistance of directed flowing water.Moreover,the 2D structure and the flowing water also provide an opportunity to convert waste solar heat into electricity in the evaporator based on the seebeck effect,ensuring simultaneous freshwater production and power generation.It is believed that this work provides insights into design-ing hybrid systems with high evaporation rate,salt resistance,and electricity generation.
查看更多>>摘要：Electrolyte solvents have a critical impact on the design of high performance and safe batteries.Gutmann's donor number(DN)and acceptor number(AN)values are two important parameters to screen and design superior electrolyte solvents.However,it is more time-consuming and expensive to obtain DN and AN values through experimental measurements.Therefore,it is essential to develop a method to pre-dict DN and AN values.This paper presented the prediction models for DN and AN based on molecular structure descriptors of solvents,using four machine learning algorithms such as CatBoost(Categorical Boosting),GBRT(Gradient Boosting Regression Tree),RF(Random Forest)and RR(Ridge Regression).The results showed that the DN and AN prediction models based on CatBoost algorithm possesses satis-factory prediction ability,with R2 values of the testing set are 0.860 and 0.96.Moreover,the study ana-lyzed the molecular structure parameters that impact DN and AN.The results indicated thatTDB02m(3D Topological distance based descriptors-lag 2 weighted by mass)had a significant effect on DN,while HATS1s(leverage-weighted autocorrelation of lag 1/weighted by I-state)plays an important role in AN.The work provided an efficient approach for accurately predicting DN and AN values,which is useful for screening and designing electrolyte solvents.
查看更多>>摘要：The proper bandgap and exceptional photostability enable CsPbl3 as a potential candidate for indoor pho-tovoltaics(IPVs),but indoor power conversion efficiency(PCE)is impeded by serious nonradiative recom-bination stemming from challenges in incomplete DMAPbI3 conversion and lattice structure distortion.Here,the coplanar symmetric structure of hexyl sulfide(HS)is employed to functionalize the CsPbI3 layer for fabricating highly efficient IPVs.The hydrogen bond between HS and DMAI promotes the conversion of DMAPbI3 to CsPbI3,while the coplanar symmetric structure enhances crystalline order.Simultaneously,surface sulfidation during HS-induced growth results in the in situ formation of PbS,spontaneously creating a CsPbI3 N-P homojunction to enhance band alignment and carrier mobility.As a result,the CsPbI3&HS devices achieve an impressive indoor PCE of 39.90％(Pin:334.6 μW cm-2,Pout:133.5 μW cm-2)under LED@2968 K,1062 lux,and maintain over 90％initial PCE for 800 h at～30％air ambient humidity.
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