查看更多>>摘要：Hydrogen sulfide(H2S)not only presents significant environmental concerns but also induces severe cor-rosion in industrial equipment,even at low concentrations.Among various technologies,the selective oxidation of hydrogen sulfide(SOH2S)to elemental sulfur(S)has emerged as a sustainable and environ-mentally friendly solution.Due to its unique properties,iron oxide has been extensively investigated as a catalyst for SOH2S;however,rapid deactivation has remained a significant drawback.The causes of iron oxide-based catalysts deactivation mechanisms in SOH2S,including sulfur or sulfate deposition,the transformation of iron species,sintering and excessive oxygen vacancy formation,and active site loss,are thoroughly examined in this review.By focusing on the deactivation mechanisms,this review aims to provide valuable insights into enhancing the stability and efficiency of iron-based catalysts for SOH2S.
查看更多>>摘要：Ni-rich layered oxides are potential cathode materials for next-generation high energy density Li-ion bat-teries due to their high capacity and low cost.However,the inherently unstable surface properties,including high levels of residual Li compounds,dissolution of transition metal cations,and parasitic side reactions,have not been effectively addressed,leading to significant degradation in their electrochemical performance.In this study,we propose a simple and effective lactic acid-assisted interface engineering strategy to regulate the surface chemistry and properties of Ni-rich LiNi0.8Co0.1Mn0.1O2 cathode.This novel surface treatment method successfully eliminates surface residual Li compounds,inhibits struc-tural collapse,and mitigates cathode-electrolyte interface film growth.As a result,the lactic acid-treated LiNi0.8Co0.1Mn0.1O2 achieved a remarkable capacity retention of 91.7％after 100 cycles at 0.5 C(25 ℃)and outstanding rate capability of 149.5 mA h g-1 at 10C,significantly outperforming the pristine material.Furthermore,a pouch-type full cell incorporating the modified LiNi0.8Co0.1Mn0.1O2 cathode demonstrates impressive long-term cycle life,retaining 81.5％of its capacity after 500 cycles at 1 C.More importantly,the thermal stability of the modified cathode is also dramatically improved.This study offers a valuable surface modification strategy for enhancing the overall performance of Ni-rich cathode materials.
查看更多>>摘要：The development of rechargeable magnesium(Mg)batteries is of practical significance to upgrade the electric energy storage devices due to exceptional capacity and abundant resources of Mg-metal anode.However,the reversible Mg electrochemistry suffers from unsatisfied rate capability and lifespan,mainly caused by non-uniform distribution of electrodeposits.In this work,a fresh design concept of three-dimensional carbon cloths scaffolds is proposed to overcome the uncontrollable Mg growth via homog-enizing electric field and improving magnesiophilicity.A microscopic smooth and nitrogen-containing defective carbonaceous layer is constructed through a facile pyrolysis of ZIF8 on carbon cloths.As revealed by finite element simulation and DFT calculation results,the smooth surface endows with uni-form electric field distribution and simultaneously the nitrogen-doping species enable good magnesio-philicity of scaffolds.The fine and uniform Mg nucleus as well as the inner electrodeposit behavior are also disclosed.As a result,an exceptional cycle life of 500 cycles at 4.0 mA cm-2 and 4.0 mA h cm-2 is firstly realized to our best knowledge.Besides,the functional scaffolds can be cycled for over 2200 h at 2.0 mA cm-2 under a normalized capacity of 5.0 mA h cm-2,far exceeding previous results.This work offers an effective approach to enable the full potential of carbon cloths-based scaffolds towards metal storage for next generation battery applications.
查看更多>>摘要：Carbon capture,utilization and storage(CCUS)is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO2 adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen uti-lization,specifically in the water gas shift,steam reforming and gasification processes.These processes are crucial for achieving carbon neutrality.While laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial environments remains challenging,impeding the commercialization process.This review aims to critically summarize the recent research progress made in intermediate-temperature(200-400 ℃)solid CO2 adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application scenarios.Additionally,we provide an overview of laboratory-level advanced technologies specifically tailored for industrial applications.Furthermore,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale implementation.The insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial applications.By promoting advances in the application of solid adsorbents,we strive to facilitate the ulti-mate goal of achieving carbon neutrality.
查看更多>>摘要：Sodium with low cost and high abundance is considered as a substitute element of lithium for batteries and supercapacitors,which need the appropriate host materials to accommodate the relatively large Na+ions.Compared to Li+storage,Na+storage makes higher demands on the structural optimization of perovskite bismuth ferrite(BiFeO3).We propose a novel strategy of defect engineering on BiFeO3 through Na and V codoping for high-efficiency Na+storage,to reveal the roles of oxygen vacancies and V ions played in the enhanced electrochemical energy storage performances of Na-ion capacitors.The formation of the oxygen vacancies in the Na and V codoped BiFeO3(denoted as NV-BFO),is promoted by Na doping and suppressed by V doping,which can be demonstrated by XPS and EPR spectra.By the first-principles calculations,the oxygen vacancies and V ions in NV-BFO are confirmed to substantially lower the Na+migration energy barriers through the space and electric field effects,to effectively promote the Na+trans-port in the crystals.Electrochemical kinetic analysis of the NV-BFO//NV-BFO capacitors indicates the dom-inant capacitive-controlled capacity,which depends on fast Na+deintercalation-intercalation process in the NV-BFO electrode.The NV-BFO//NV-BFO capacitors open up a new avenue for developing high-performance Na-ion capacitors.
查看更多>>摘要：Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emis-sions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU)represents one of the approaches and thermochemical CO2 splitting driven by thermal energy is a subset of the CCU,which converts the captured CO2 into CO and makes it possible to achieve closed-loop carbon recircula-tion.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advance-ments in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to pro-vide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and com-posite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO2 splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.
查看更多>>摘要：Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tol-erance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and corrosion.Here,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater electrolysis.Such a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl-,resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing test.Further,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V vs.RHE,a potential that is far beyond the ther-modynamic potential of chlorine ion oxidation.This concept and approach to reasonably designing weak-nucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the develop-ment of green hydrogen technique.
查看更多>>摘要：Inverted perovskite solar cells(PSCs)have attracted broad research and industrial interest owing to their suppressed hysteresis,cost-effectiveness,and easy-fabrication.However,the issue of non-radiative recombination losses at the n-type interface between the perovskite and fullerene has impeded further improvement of photovoltaic performance.Here,we modify the n-type interface of FAPbI3 perovskite films by constructing a stereochemical two-dimensional(2D)perovskite interlayer,in which the organic cations comprise both pyridine and ammonium groups.The pyridine N donor can create stable bonding with the surface-uncoordinated Pb on the perovskite,thereby passivating the shallow-level defects and enhancing the air stability of the film.Furthermore,the pyridine N donor also offers a positive polar interface to decrease the surface work function of the perovskite film,enabling n-type modification.Ultimately,we employ a p-i-n photovoltaic(PV)device with the positive dipole interlayer at perovskite/fullerene contact and achieve remarkable photoelectric conversion efficiency(PCE)of 22.0％.
查看更多>>摘要：Lead iodide(PbI2)is a vital raw material for preparing perovskite solar cells(PSCs),and it not only takes part in forming the light absorption layer but also remains in the grain boundary as a passivator.In other words,the PbI2 content in the precursor and as formed film will affect the efficiency and stability of the PSCs.With moderate residual PbI2,it passivates the bulk/surface defects of perovskite,reduces the inter-facial recombination,promotes the perovskite stability,minimizes the device hysteresis,and so on.Deficient PbI2 residue will reduce the interfacial passivation effect and device performance.In addition to facilitating the non-radiative recombination,over PbI2 residue can also lead to electronic insulation in the grain boundary and deteriorate the device performance.However,the impact and regulation of PbI2 residue on the device performance and stability is still not fully understood.Herein,a comprehen-sive and detailed review is presented by discussing the PbI2 residue impact and its regulation strategies(i.e.,elimination,facilitation and conversion of the residue PbI2)to manipulate the PbI2 content,distri-bution and forms.Finally,we also show future outlooks in this field,with an aim to help further the pro-gression of high-efficiency and stable PSCs.
查看更多>>摘要：Dual-atom catalysts(DACs)afford promising potential for oxygen reduction electrocatalysis due to their high atomic efficiency and high intrinsic activity.However,precise construction of dual-atom sites remains a challenge.In this work,a post-modification strategy is proposed to precisely fabricate DACs for oxygen reduction electrocatalysis.Concretely,a secondary metal precursor is introduced to the pri-mary single-atom sites to introduce direct metal-metal interaction,which ensures the formation of desired atom pair structure during the subsequent pyrolysis process and allows for successful construc-tion of DACs.The as-prepared FeCo-NC DAC exhibits superior oxygen reduction electrocatalytic activity with a half-wave potential of 0.91 V vs.reversible hydrogen electrode.Zn-air batteries equipped with the FeCo-NC DAC demonstrate higher peak power density than those with the Pt/C benchmark.More impor-tantly,this post-modification strategy is demonstrated universal to achieve a variety of dual-atom sites.This work presents an effective synthesis methodology for precise construction of catalytic materials and propels their applications in energy-related devices.
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