查看更多>>摘要：Metal-organic frameworks(MOFs)possess a distinct advantage over conventional heterogeneous photo-catalysts because of their carefully defined architecture and particular pores,which facilitate the targeted incorporation of other efficient cocatalysts or semiconductor materials.The integration of MOFs with other materials has resulted in significant breakthroughs,as the coupled materials improve the perfor-mance due to the combined effect.The unique MOF structures allow them to host foreign materials,which results in harvesting the visible region of the solar spectrum and effectively mitigating charge recombination by promoting charge separation.The review presents an evaluation of the latest develop-ments in the utilization of surface and/or pore chemistry of MOF-supported heterojunctions for photocat-alytic green-hydrogen generation with a basic understanding of the mechanism involved.The review begins with the basic principles of photocatalysis,the significance of MOFs,their optical properties,the methods used for synthesizing MOFs,and their coordination with other inorganic and polymeric materials.Furthermore,methods to increase photocatalytic H2 evolution using MOF-supported hetero-junction have been proposed as standard practice.Lastly,to address environmental challenges,we high-light the future potential of MOF-supported heterojunctions for use in green-energy production.We hope that this review provides guidance to researchers in the development of effective heterojunctions based on MOFs to address challenges in energy applications and catalytic processes.
查看更多>>摘要：While reliance on renewable energy resources has become a reality,there is still a need to deploy greener and more sustainable methods in order to achieve sustainable development goals.Indeed,green hydro-gen is currently believed to be a reliable solution for global warming and the pollution challenges arising from fossil fuels,making it the resilient fuel of the future.However,the sustainability of green hydrogen technologies is yet to be achieved.In this context,generation of green hydrogen with the aid of deep eutectic solvents(DESs)as green mixtures has been demonstrated as a promising research area.This sys-tematic review article covers green hydrogen generation through water splitting and biomass fermenta-tion when DESs are utilized within the generation process.It also discusses the incorporation of DESs in fuel cell technologies.DESs can play a variety of roles such as solvent,electrolyte,or precursor;colloidal suspension and reaction medium;galvanic replacement,shape-controlling,decoration,or extractive agent;finally oxidant.These roles are relevant to several methods of green hydrogen generation,includ-ing electrocatalysis,photocatalysis,and fermentation.As such,it is of utmost importance to screen poten-tial DES formulations and determine how they can function in and contribute throughout the green hydrogen mobility stages.The realization of super green hydrogen generation stands out as a pivotal milestone in our journey towards achieving a more sustainable form of development;DESs have great potential in making this milestone achievable.Overall,incorporating DESs in hydrogen generation con-stitutes a promising research area and offers potential scalability for green hydrogen production,storage,transport,and utilization.
查看更多>>摘要：Surface reconstruction yields real active species in electrochemical oxygen evolution reaction(OER)con-ditions;however,rationally regulating reconstruction in a targeted manner for constructing highly active OER electrocatalysts remains a formidable challenge.Here,an electrochemical activation strategy with selective etching was utilized to guide the reconstruction process of a hybrid cobalt-molybdenum oxide(CoMoO4/Co3O4@CC)in a favorable direction to improve the OER performance.Both in-situ Raman and multiple ex-situ characterization tools demonstrate that controlled surface reconstruction can be easily achieved through Mo etching,with the formation of a dynamically stable amorphous-crystalline heterostructure.Theoretical calculations together with experimental results reveal that the synergistic effects between amorphous CoOOH and crystalline Co3O4 are crucial in enhancing the catalytic perfor-mance.Consequently,the reconstructed CoMoO4/Co3O4@CC exhibits a low overpotential of 250 mV to achieve a current density of 10 mA cm-2 in 1 M KOH,and more importantly it can be practiced in elec-trolytic water splitting and rechargeable zinc-air batteries devices,achieving ultra-long stability for over 500 and 1200 h,respectively.This work provides a promising route for the construction of high-performance electrocatalysts.
查看更多>>摘要：Inadequate interfacial contact between lithium and solid-state electrolytes(SSEs)leads to elevated impe-dance and the growth of lithium dendrites,presenting significant obstacles to the practical viability of solid-state batteries(SSBs).To ameliorate interfacial contact,optimizing the surface treatment of SSEs has been widely adopted.However,the formation of LiCl through acid treatment,an equally crucial factor impacting SSB performance,has received limited attention,leaving its underlying mechanism unclear.Our study aims to shed light on SSE characteristics following LiCl formation and the removal of Li2CO3 through acid treatment.We seek to establish quantifiable links between SSE surface structure and SSB performance,focusing on interfacial resistance,current distribution,critical current density(CCD),and lithium deposition.The formation of LiCl,occurring as Li2CO3 is removed through acid treatment,effec-tively mitigates lithium dendrite formation on SSE surfaces.This action inhibits electron injection and reduces the diffusion rate of Li atoms.Simultaneously,acid treatment transforms the SSE surface into a lithiophilic state by eliminating surface Li2CO3.Consequently,the interfacial resistance between lithium and SSEs substantially decreases from 487.67 to 35.99 Ω cm2 at 25 ℃.This leads to a notably high CCD of 1.3 mA cm-2 and a significantly extended cycle life of 1,000 h.Furthermore,in full SSBs incorporating LiCoO2 cathodes and acid-treated garnet SSEs,we observe exceptional cyclability and rate capability.Our findings highlight that acid treatment not only establishes a fundamental relationship between SSE surfaces and battery performance but also offers an effective strategy for addressing interfacial chal-lenges in SSBs.
查看更多>>摘要：Sodium metal batteries(SMBs)have attracted increasing attention over time due to their abundance of sodium resources and low cost.However,the widespread application of SMBs as a viable technology remains a great challenge,such as uneven metallic deposition and dendrite formation during cycling.Carbon skeletons as sodiophilic hosts can alleviate the dendrite formation during the plating/stripping.For the carbon skeleton,how to rationalize the design sodiophilic interfaces between the sodium metal and carbon species remains key to developing desirable Na anodes.Herein,we fabricated four kinds of structural features for carbon skeletons using conventional calcination and flash Joule heating.The roles of conductivity,defects,oxygen content,and the distribution of graphite for the deposition of metallic sodium were discussed in detail.Based on interface engineering,theJ1600 electrode,which has abundant Na-C species on its surface,showed the highest sodiophilic.There are uniform and rich F-Na species dis-tributed in the inner solid electrolyte interface layer.This study investigated the different Na-deposition behavior in carbon hosts with distinct graphitic arrangements to pave the way for designing and optimiz-ing advanced electrode materials.
查看更多>>摘要：Ultra-long n-alkanes are highly valuable in both scientific research and as major constituents of specialty high-melting-point waxes.Unlike conventional methods(e.g.,Fischer-Tropsch(FT),ethylene oligomer-ization,and polyethylene cracking)typically resulting in wide n-alkane distributions,the elaborate design strategy presented herein allows the direct synthesis of pure,long n-alkanes using a modular splicing method with acetone,furfural,and fatty acid anhydrides or acyl chlorides as bio-blocks.The herein approach is based on a simple four-step catalytic reaction scheme involving C-C chain elongation and C-O bond activation.The synthesized pure n-alkanes had a carbon chain length as high as C49(total yield of 49％).The synthesis approach also allows to selectively prepare n-alkanes with even and odd car-bon numbers ranging from C15 to C49.This process represents a great breakthrough in the synthesis of long-chain pure n-alkanes,surpassing the carbon number limitations reported in previous methodologies.
James CloseJonathan E.BarnardY.M.John ChewSemali Perera...
422-439页
查看更多>>摘要：The integration of battery energy storage systems(BESS)throughout our energy chain poses concerns regarding safety,especially since batteries have high energy density and numerous BESS failure events have occurred.Wider spread adoption will only increase the prevalence of these failure events unless there is a step change in the management and design of BESS.To understand the causes of failure,the main challenges of BESS safety are summarised.BESS consequences and failure events are discussed,including specific focus on the chain of events causing thermal runaway,and a case study of a BESS explo-sion in Surprise Arizona is analysed.Based on the technology and past events,a paradigm shift is required to improve BESS safety.In this review,a holistic approach is proposed.This combines currently adopted approaches including battery cell testing,lumped cell mathematical modelling,and calorimetry,along-side additional measures taken to ensure BESS safety including the requirement for computational fluid dynamics and kinetic modelling,assessment of installation level testing of the full BESS system and not simply a single cell battery test,hazard and layers of protection analysis,gas chromatography,and com-position testing.The holistic approach proposed in this study aims to address challenges of BESS safety and form the basis of a paradigm shift in the safety management and design of these systems.
查看更多>>摘要：Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high the-oretical specific capacities(～660 mA h g-1)and suitable voltage platforms.However,severe capacity fad-ing caused by huge volume change and limited ion transportation hinders their practical applications.Recently,strategies for controlling the morphologies of Sb-based materials to improve the electrochem-ical performances have been proposed.Among these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion diffusion.Nevertheless,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,espe-cially how to obtain large-scale 2D-Sb materials.Herein,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is provided.This method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon layer.Compared to the reported methods,it is simpler,more efficient,and conducive to the production of com-posite nanosheets with uniform thickness(3-4 nm).The 2D-Sb@NC nanosheet anode delivers an extre-mely high capacity of 504.5 mA h g-1 at current densities of 100 mA g-1 and remains stable for more than 200 cycles.Through characterizations and molecular dynamic simulations,how potassium storage kinet-ics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are provided.These findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.
查看更多>>摘要：High-energy density lithium-ion batteries(LIBs)with layered high-nickel oxide cathodes(LiNixCoyMn1-x-yO2,x ≥ 0.8)show great promise in consumer electronics and vehicular applications.However,LiNixCoyMn1-x-yO2 faces challenges related to capacity decay caused by residual alkalis owing to high sensitivity to air.To address this issue,we propose a hazardous substances upcycling method that fundamentally mitigates alkali content and concurrently induces the emergence of an anti-air-sensitive layer on the cathode surface.Through the neutralization of polyacrylic acid(PAA)with residual alkalis and then coupling it with 3-aminopropyl triethoxysilane(KH550),a stable and ion-conductive cross-linked polymer layer is in situ integrated into the LiNi0.89Co0.06Mn0.05O2(NCM)cathode.Our characteri-zation and measurements demonstrate its effectiveness.The NCM material exhibits impressive cycling performance,retaining 88.4％of its capacity after 200 cycles at 5 C and achieving an extraordinary specific capacity of 170.0 mA h g-1 at 10 C.Importantly,this layer on the NCM efficiently suppresses unfavorable phase transitions,severe electrolyte degradation,and CO2 gas evolution,while maintaining commend-able resistance to air exposure.This surface modification strategy shows widespread potential for creat-ing air-stable LiNixCoyMn1-x-yO2 cathodes,thereby advancing high-performance LIBs.
查看更多>>摘要：Ammonia(NH3)is a multifunctional compound that is an important feedstock for the agricultural and pharmaceutical industries and attractive energy storage medium.At present,NH3 synthesis is highly dependent on the conventional Haber-Bosch process that operates under harsh conditions,which con-sumes large quantities of fossil fuels and releases a large amount of carbon dioxide.As an alternative,electrosynthesis is a prospective method for producing NH3 under normal temperature and pressure con-ditions.Although electrocatalytic nitrogen reduction to ammonia has attracted considerable attentions,the low solubility of N2 and high N=N cracking energy render the achievements of high NH3 yield rate and Faradaic efficiency difficult.Nitrate and nitrite(NOx-)are common N-containing pollutants.Due to their high solubilities and low dissociation energy of N=O,NOx-are ideal raw materials for NH3 pro-duction.Therefore,electrocatalytic NOx-reduction to NH3(eNOxRR)is a prospective strategy to simulta-neously realise environmental protection and NH3 synthesis.This review offers a comprehensive understanding of the thriving eNOxRR under ambient conditions.At first,the popular theory and mech-anism of eNOxRR and a summary of the measurement system and evaluation criteria are introduced.Thereafter,various strategies for developing NOx-reduction catalysts are systematically presented and discussed.Finally,the challenges and possible prospects of electrocatalytic NOx-reduction are outlined to facilitate energy-saving and environmentally friendly large-scale synthesis of NH3 in the future.
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