With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power ...With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.展开更多
Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling technique...Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling techniques is increasingly compromised by their high energy consumption and secondary pollution,rendering them less responsive to greener and more sustainable requirement of rapid development.Thus,the direct recycling process emerged and was considered as a more expedient and convenient method of recycling compared to the conventional recycling modes that are currently in study.However,due to the reliance on the indispensable sintering process,direct recycling still faces considerable challenges,motivating researchers to explore faster,greener,and more cost-effective strategies for LIBs recycling,Inspiringly,Joule heating recycling(JHR),an emerging technique,offers rapid,efficient impurity removal and material regeneration with minimal environmental impact,addressing limitations of existing methods.This method reduces the time for direct recycling of spent LIBs by a factor of at least three orders of magnitude and exhibits significant potential for future industrial production.Unfortunately,due to the lack of systematic organization and reporting,this next generation approach to direct recycling of spent LIBs has not yet gained much interest.To facilitate a more profound comprehension of rising flash recycling strategy,in this study,JHR is distinguished into two distinctive implementation pathways(including flash Joule heating and carbon thermal shock),designed to accommodate varying pretreatment stages and diverse spent LIBs materials.Subsequently,the advantages of the recently developed JHR of spent LIBs in terms of material performance,environmental friendliness,and economic viability are discussed in detail.Ultimately,with the goal of achieving more attractive society effects,the future direction of JHR of spent LIBs and its potential for practical application are proposed and envisaged.展开更多
Cold plasma-assisted catalytic upcycling of polyolefin wastes integrated with CO_(2)into value-added chemicals is a promising solution for mitigating the global carbon emissions and fossil energy crisis,but still chal...Cold plasma-assisted catalytic upcycling of polyolefin wastes integrated with CO_(2)into value-added chemicals is a promising solution for mitigating the global carbon emissions and fossil energy crisis,but still challenging due to the complexity of products and low energy efficiency.Given this,a novel one-stage process of cold plasma coupled with Ga-modified hierarchical H-ZSM-5(Ga/Hie-ZSM-5)catalyst for polyolefins upgrading was designed with polyolefins followed by the catalysts within the plasma region,which facilitated the upcycling of polyolefins to light olefins and CO_(2)activation by plasma,and thereby the enhanced synergy between cold plasma and catalysts for aromatics production.At an input power of ca.45 W without external heating,the low-density polyethylene(LDPE)waste was completely converted with the assistance of CO_(2)and the yield of oil products over the Ga/Hie-ZSM-5 catalyst was highly up to 62.2 wt%,with nearly 100% selectivity of aromatics.Meanwhile,the degradation efficiency of LDPE and the energy efficiency could reach 2.5 g_(LDPE)·g_(cat)^(-1)·h^(-1)and 55.56 g_(LDPE)·g_(cat)^(-1)·kW^(-1)h^(-1),respectively.Mechanism investigation revealed that the plasma and CO_(2)synergistically affect the primary cracking of LDPE,forming a primary product enriched in olefins and a small amount of CO.Subsequently,the produced olefins intermediates were further aromatized via cyclizationdehydrogenation route on the Ga/Hie-ZSM-5 catalyst with assistance of CO_(2)under the synergistic effect of plasma-catalysis.This work offers a feasible strategy to improve the yield of aromatic products for the plasma-catalytic upcycling of polyolefins and CO_(2)at ambient pressure without any external heating.展开更多
Chemical recycling/upcycling of plastics has emerged as one of the most promising strategies for the plastic circular economy,enabling the depolymerization and functionalization of plastics into valuable monomers and ...Chemical recycling/upcycling of plastics has emerged as one of the most promising strategies for the plastic circular economy,enabling the depolymerization and functionalization of plastics into valuable monomers and chemicals.However,studies on the depolymerization and functionalization of challenging super engineering plastics have remained in early stage and underexplored.In this review,we would like to discuss the representative accomplishments and mechanism insights on chemical protocols achieved in depolymerization of super engineering plastics,especially for poly(phenylene sulfide)(PPS),poly(aryl ether)s including poly(ether ether ketone)(PEEK),polysulfone(PSU),polyphenylsulfone(PPSU)and polyethersulfone(PES).We anticipate that this review will provide an overall perspective on the current status and future trends of this emerging field.展开更多
Current ever-accumulating plastic waste can be considered a significant carbon resource for energy conversion and chemical production.The development of new approaches for upcycling plastic waste through chemical degr...Current ever-accumulating plastic waste can be considered a significant carbon resource for energy conversion and chemical production.The development of new approaches for upcycling plastic waste through chemical degradation may enable circularity and promote closed-loop recycling of carbon sources compared to traditional recycling methods.Zeolite,a widely used solid acid catalyst with high industrial potential in petroleum and biomass refining,has been extensively studied for its role in transforming plastics.In this review,we present an overview of zeolite-based catalytic systems for the chemical recycling of plastic waste and discuss how zeolites could potentially contribute to the future development of a circular economy.To provide a comprehensive understanding,we begin with a brief introduction to zeolites,analyzing their key features and exploring their opportunities as well as challenges in processing plastic waste.Subsequently,we delve into the chemistry of catalytic cracking and tandem catalysis using zeolite-based catalysts on plastics.Overall,we emphasize the importance of intelligent catalyst design and lower-energy pathways to incentivize plastic upcycling while alleviating the burden caused by waste plastics.展开更多
Paired electrolysis of waste feedstocks holds an energy-efficient alternative for chemical production;however,the sluggish anodic oxidation limited the total efficiency under larger current density.Herein,we construct...Paired electrolysis of waste feedstocks holds an energy-efficient alternative for chemical production;however,the sluggish anodic oxidation limited the total efficiency under larger current density.Herein,we constructed ultralow-coordinated Ni species with Ni–O coordination number of∼3 via a hydrothermal synthesis-sulfidation-annealing process and electrochemical activation and demonstrated the vital role in accelerating the proton deintercalation and reactive oxygen intermediate·OH formation during electro-reforming polyethylene terephthalate hydrolysate(POR).The target catalyst NiCoSx/NF afforded a high formate productivity of 7.4 mmol cm^(−2)h^(−1)at∼600 mA cm^(−2)with a formate Faradic efficiency(FE_(formate))of 92.4%in POR and maintained a FE_(formate)of∼90%for 100 h at 2 A in a membrane electrode assembly electrolyzer.Coupling POR on NiCoSx/NF with carbon dioxide reduction reaction on oxygen vacancies enriched Vo-BiSnO reached effective concurrent formate production with 172.7%of FE_(formate)at 500 mA cm^(−2)and long-term stability.Such excellent performance shows the great prospect of electrocatalyst design by regulating the local metal environment.展开更多
The unprecedented growth of electric vehicles featuring lithium-ion batteries has led to a significant increase in the amount of waste generated,posing pressing waste management challenges for both industry professio ...The unprecedented growth of electric vehicles featuring lithium-ion batteries has led to a significant increase in the amount of waste generated,posing pressing waste management challenges for both industry professio nals and environmental regulators.To address these issues,conventio nal pyrometallurgical,hydrometallurgical,and direct recycling methods are commonly employed to promote sustainable battery development.However,these methods are often hindered by laborious purification processes and the generation of low-profit products such as Li_(2)CO_(3),CoSO_(4),NiSO_(4),etc.Herein,an upcycling technology involving a low-temperature solid-to-solid reaction and water leaching procedures is introduced to transform spent LiCoO_(2)cathode materials into value-added cobalt sulfide-based electrocatalysts.The regenerated electrocatalysts exhibit exceptional performance in the oxygen evolution reaction,surpassing that of the benchmark RuO_(2)catalyst.This proposed upcycling method provides researchers with an alternative way to convert the metallic components of waste lithium-ion batteries into high-value Co-,Ni-,Fe-,and Mn-based catalysts.展开更多
Poly(ethylene glycol-co-1,4-cyclohexanedimethanol terephthalate)(PETG)possesses excellent properties and stability than traditional poly(ethylene terephthalate)(PET).However,the production and application of PETG are ...Poly(ethylene glycol-co-1,4-cyclohexanedimethanol terephthalate)(PETG)possesses excellent properties and stability than traditional poly(ethylene terephthalate)(PET).However,the production and application of PETG are restricted by the expensive monomer(1,4-cyclohexanedimethanol,CHDM).Direct upgrading of waste PET to dimethyl cyclohexane-1,4-dicarboxylate(DMCD)can promote the production of CHDM in large scale.In this work,a bifunctional Ru/UiO-66_(def)-SO_(3)H catalyst was synthesized and utilized in coupled methanolysis(of waste PET to dimethyl terephthalate(DMT))and hydrogenation(of DMT to DMCD)under mild condition.Characterizations revealed that Ru/UiO-66_(def)-SO_(3)H possessed mesopores(dominant channels of 2.72 and 3.44 nm),enlarged surface area(998 m^(2)·g^(–1)),enhanced acidity(580μmol·g^(–1)),and Ru nanoparticles(NPs)dispersed highly(45.1%)compared to those of Ru/UiO-66.These combined advantages could accelerate the methanolysis and hydrogenation reactions simultaneously,promoting the performance of direct upgrading of PET to DMCD in one pot.In particular,the conversion of PET and yield of DMCD over Ru/UiO-66_(def)-SO_(3)H reached 100%and 97.7%at 170℃and 3 MPa H_(2)within 6 h.Moreover,Ru/UiO-66_(def)-SO3H was also capable for the upcycling of waste PET-based products including beverage bottles,textile fiber and packaging film to DMCD.展开更多
Poly(butylene adipate-co-terephthalate)(PBAT),a widely studied biodegradable material,has not effectively addressed the problem of plastic waste.Taking into consideration the cost-effectiveness,upcycling PBAT should t...Poly(butylene adipate-co-terephthalate)(PBAT),a widely studied biodegradable material,has not effectively addressed the problem of plastic waste.Taking into consideration the cost-effectiveness,upcycling PBAT should take precedence over direct composting degradation.The present work adopts a chain breaking-crosslinking strategy,upcycling PBAT into dual covalent adaptable networks(CANs).During the chainbreaking stage,the ammonolysis between PBAT and polyethyleneimine(PEI)established the primary crosslinked network.Subsequently,styrene maleic anhydride copolymer(SMA)reacted with the hydroxyl group,culminating in the formation of dual covalent adaptable networks.In contrast to PBAT,the PBAT-dual-CANs exhibited a notable Young's modulus of 239 MPa,alongside an inherent resistance to creep and solvents.Owing to catalysis from neighboring carboxyl group and excess hydroxyl groups,the PBAT-dual-CANs exhibited fast stress relaxation.Additionally,they could be recycled through extrusion and hot-press reprocessing,while retaining their biodegradability.This straightforward strategy offers a solution for dealing with plastic waste.展开更多
Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only ...Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only 9%,has led to a monumental environmental crisis.Plastic recycling has emerged as a vital response to this crisis,offering sustainable solutions to mitigate its environmental impact.Among these recycling efforts,plastic upcycling has garnered attention,which elevates discarded plastics into higher-value products.Here,electrocatalytic and photoelectrocatalytic treatments stand at the forefront of advanced plastic upcycling.Electrocatalytic or photoelectrocatalytic treatments involve chemical reactions that facilitate electron transfer through the electrode/electrolyte interface,driven by electrical or solar energy,respectively.These methods enable precise control of chemical reactions,harnessing potential,current density,or light to yield valuable chemical products.This review explores recent progress in plastic upcycling through electrocatalytic and photoelectrocatalytic pathways,offering promising solutions to the plastic waste crisis and advancing sustainability in the plastics industry.展开更多
The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable development.Compared with the degraded cathode,spent anode graphite ofte...The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable development.Compared with the degraded cathode,spent anode graphite often has a relatively intact structure with few defects after long cycling.Yet,most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex,have low efficiency,and fail in performance restoration.Herein,we propose a fast,efficient,and“intelligent”strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation.Using Sn as a nanoscale healant,we used rapid heating(~50 ms)to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects(~5.84 eV/atom),thus simultaneously achieving Sn dispersion and graphite remediation.As a result,the regenerated graphite showed enhanced capacity and cycle stability(458.9 mAh g^(−1) at 0.2 A g^(−1) after 100 cycles),superior to those of commercial graphite.Benefiting from the self‐adaption of Sn dispersion,spent graphite with different degrees of defects can be regenerated to similar structures and performance.EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption(~99%reduction)and near‐zero CO_(2) emission,and yield much higher profit than hydrometallurgy,which opens a new avenue for direct upcycling of spend graphite in an efficient,green,and profitable manner for sustainable battery manufacture.展开更多
With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions ...With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.展开更多
The conversion of waste polylactic acid(PLA)plastics into high-value-added chemicals through electrochemical methods is a promising and sustainable approach.However,developing efficient and highly selective catalysts ...The conversion of waste polylactic acid(PLA)plastics into high-value-added chemicals through electrochemical methods is a promising and sustainable approach.However,developing efficient and highly selective catalysts for lactic acid oxidation reaction(LAOR)and understanding the reaction process are challenging.Here,we report the electrooxidation of waste PLA to acetate at a high current density of 100 mA cm-2 with high Faraday efficiency(~95%)and excellent stability(>100 h)over a nickel selenide nanosheet catalyst.In addition,a total Faraday efficiency of up to 190%was achieved for carboxylic acids,including acetic acid and formic acid,by coupling with the cathodic CO_(2) reduction reaction.In situ experimental results and theoretical simulations revealed that the catalytic activity center of LAOR was dynamically formed NiOOH species,and the surface-adsorbed SeO_(x) species accelerated the formation of Ni~(3+)species,thus promoting catalytic activity.The mechanism of lactic acid electrooxidation was further elucidated.Lactic acid was dehydrogenated to produce pyruvate first and then formed CH_3CO due to preferential C-C bond cleavage,resulting in the presence of acetate.This work demonstrated a sustainable method for recycling waste PLA and CO_(2) into high-value-added products.展开更多
The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-...The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.展开更多
As global municipal solid waste(MSW)quantities continue to escalate,serious socio-environmental challenges arise,necessitating innovative solutions.Waste-to-hydrogen(WTH)via two-stage gasification-reforming(TSGR)prese...As global municipal solid waste(MSW)quantities continue to escalate,serious socio-environmental challenges arise,necessitating innovative solutions.Waste-to-hydrogen(WTH)via two-stage gasification-reforming(TSGR)presents an emergent technology for MSW upcycling,offering to ease waste management burdens and bolster the burgeoning hydrogen economy.Despite early initiatives to advance TSGR technology,a cohesive and critical analysis of cutting-edge knowledge and strategies to enhance hydrogen production remains lacking.This review aggregates literature on MSW upcycling to hydrogen via TSGR,with a focus on optimizing process control and catalytic efficiency.It underscores technological avenues to augment hydrogen output,curtail catalyst costs,and refine system performance.Particularly,the review illuminates the potential for integrating chemical and calcium looping into TSGR processes,identifying opportunities,and pinpointing challenges.The review concludes with a summary of the current state of techno-economic analysis for this technology,presenting outstanding challenges and future research directions,with the ultimate goal of transitioning WTH from theoretical to practical application.展开更多
基金financially supported by the National Key Research and Development Program of China(2023YFB3809300)。
文摘With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.
基金financially supported by the National Key Research and Development Program of China(No.2023YFC3904800)the National Outstanding Young Scientists Fund(No.5a2125002)+7 种基金the National Science Foundation of China(No.22476073)the Key Project of Jiangxi Provincial Research and Development Program(Nos.20223BBG74006 and 20243BBI91001)the China Postdoctoral Science Foundation(No.2024M751282)the “Thousand Talents Program”of Jiangxi Province(S_(2)021GDQN2161)the Key Project of Ganzhou City Research and Development Program(No.2023PGX17350)the Science&Technology Talent Lifting Project of Hunan Province(No.2022TJ-N16)the Natural Science Foundation of Hunan Province China(No.2024JJ4022,2023JJ30277)the Open-End Fund for National-Local Joint Engineering Research Center of Heavy Metals Pollutants Control and Resource Utilization(ES_(2)02480184)。
文摘Lithium-ion batteries(LIBs)are critical for the rapid growth of electric vehicles(EVs),but their inherent lifespan leads to numerous retirements and resource challenges.The efficacy of conventional recycling techniques is increasingly compromised by their high energy consumption and secondary pollution,rendering them less responsive to greener and more sustainable requirement of rapid development.Thus,the direct recycling process emerged and was considered as a more expedient and convenient method of recycling compared to the conventional recycling modes that are currently in study.However,due to the reliance on the indispensable sintering process,direct recycling still faces considerable challenges,motivating researchers to explore faster,greener,and more cost-effective strategies for LIBs recycling,Inspiringly,Joule heating recycling(JHR),an emerging technique,offers rapid,efficient impurity removal and material regeneration with minimal environmental impact,addressing limitations of existing methods.This method reduces the time for direct recycling of spent LIBs by a factor of at least three orders of magnitude and exhibits significant potential for future industrial production.Unfortunately,due to the lack of systematic organization and reporting,this next generation approach to direct recycling of spent LIBs has not yet gained much interest.To facilitate a more profound comprehension of rising flash recycling strategy,in this study,JHR is distinguished into two distinctive implementation pathways(including flash Joule heating and carbon thermal shock),designed to accommodate varying pretreatment stages and diverse spent LIBs materials.Subsequently,the advantages of the recently developed JHR of spent LIBs in terms of material performance,environmental friendliness,and economic viability are discussed in detail.Ultimately,with the goal of achieving more attractive society effects,the future direction of JHR of spent LIBs and its potential for practical application are proposed and envisaged.
基金financially supported by the National Key R&D Program of China(2023YFA1506602 and 2021YFA1501102)the National Natural Science Foundation of China(21932002,22276023,22402019)+1 种基金the Fundamental Research Funds for the Central Universities(DUT22LAB602)Liaoning Binhai Laboratory Project(LBLF-202306)。
文摘Cold plasma-assisted catalytic upcycling of polyolefin wastes integrated with CO_(2)into value-added chemicals is a promising solution for mitigating the global carbon emissions and fossil energy crisis,but still challenging due to the complexity of products and low energy efficiency.Given this,a novel one-stage process of cold plasma coupled with Ga-modified hierarchical H-ZSM-5(Ga/Hie-ZSM-5)catalyst for polyolefins upgrading was designed with polyolefins followed by the catalysts within the plasma region,which facilitated the upcycling of polyolefins to light olefins and CO_(2)activation by plasma,and thereby the enhanced synergy between cold plasma and catalysts for aromatics production.At an input power of ca.45 W without external heating,the low-density polyethylene(LDPE)waste was completely converted with the assistance of CO_(2)and the yield of oil products over the Ga/Hie-ZSM-5 catalyst was highly up to 62.2 wt%,with nearly 100% selectivity of aromatics.Meanwhile,the degradation efficiency of LDPE and the energy efficiency could reach 2.5 g_(LDPE)·g_(cat)^(-1)·h^(-1)and 55.56 g_(LDPE)·g_(cat)^(-1)·kW^(-1)h^(-1),respectively.Mechanism investigation revealed that the plasma and CO_(2)synergistically affect the primary cracking of LDPE,forming a primary product enriched in olefins and a small amount of CO.Subsequently,the produced olefins intermediates were further aromatized via cyclizationdehydrogenation route on the Ga/Hie-ZSM-5 catalyst with assistance of CO_(2)under the synergistic effect of plasma-catalysis.This work offers a feasible strategy to improve the yield of aromatic products for the plasma-catalytic upcycling of polyolefins and CO_(2)at ambient pressure without any external heating.
基金supported by the National Natural Science Foundation of China(Nos.22125103 and 22301077)STCSM(22JC140100)Shanghai Pujiang Program(No.22PJ1403200)。
文摘Chemical recycling/upcycling of plastics has emerged as one of the most promising strategies for the plastic circular economy,enabling the depolymerization and functionalization of plastics into valuable monomers and chemicals.However,studies on the depolymerization and functionalization of challenging super engineering plastics have remained in early stage and underexplored.In this review,we would like to discuss the representative accomplishments and mechanism insights on chemical protocols achieved in depolymerization of super engineering plastics,especially for poly(phenylene sulfide)(PPS),poly(aryl ether)s including poly(ether ether ketone)(PEEK),polysulfone(PSU),polyphenylsulfone(PPSU)and polyethersulfone(PES).We anticipate that this review will provide an overall perspective on the current status and future trends of this emerging field.
文摘Current ever-accumulating plastic waste can be considered a significant carbon resource for energy conversion and chemical production.The development of new approaches for upcycling plastic waste through chemical degradation may enable circularity and promote closed-loop recycling of carbon sources compared to traditional recycling methods.Zeolite,a widely used solid acid catalyst with high industrial potential in petroleum and biomass refining,has been extensively studied for its role in transforming plastics.In this review,we present an overview of zeolite-based catalytic systems for the chemical recycling of plastic waste and discuss how zeolites could potentially contribute to the future development of a circular economy.To provide a comprehensive understanding,we begin with a brief introduction to zeolites,analyzing their key features and exploring their opportunities as well as challenges in processing plastic waste.Subsequently,we delve into the chemistry of catalytic cracking and tandem catalysis using zeolite-based catalysts on plastics.Overall,we emphasize the importance of intelligent catalyst design and lower-energy pathways to incentivize plastic upcycling while alleviating the burden caused by waste plastics.
基金We highly thank the funding from the National Natural Science Foundation of China(grants 22222806,22178162,22072065,and 22408170)the Distinguished Youth Foundation of Jiangsu Province(BK20220053)+2 种基金the National Key Research and Development Program of China(2024YFE0206900)the Six Talent Peaks Project in Jiangsu Province(grant JNHB-035)Agency for Science,Technology and Research(A*STAR)through Low Carbon Energy Research Finding Initiative(LCERFI01-0033|U2102d2006).
文摘Paired electrolysis of waste feedstocks holds an energy-efficient alternative for chemical production;however,the sluggish anodic oxidation limited the total efficiency under larger current density.Herein,we constructed ultralow-coordinated Ni species with Ni–O coordination number of∼3 via a hydrothermal synthesis-sulfidation-annealing process and electrochemical activation and demonstrated the vital role in accelerating the proton deintercalation and reactive oxygen intermediate·OH formation during electro-reforming polyethylene terephthalate hydrolysate(POR).The target catalyst NiCoSx/NF afforded a high formate productivity of 7.4 mmol cm^(−2)h^(−1)at∼600 mA cm^(−2)with a formate Faradic efficiency(FE_(formate))of 92.4%in POR and maintained a FE_(formate)of∼90%for 100 h at 2 A in a membrane electrode assembly electrolyzer.Coupling POR on NiCoSx/NF with carbon dioxide reduction reaction on oxygen vacancies enriched Vo-BiSnO reached effective concurrent formate production with 172.7%of FE_(formate)at 500 mA cm^(−2)and long-term stability.Such excellent performance shows the great prospect of electrocatalyst design by regulating the local metal environment.
基金financial support from the National Natural Science Foundation of China(21702143,52303092)Talent Recruitment Project of Guangdong Province(No.2023QN10X078)+1 种基金Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(No.YPML-2023050278)Guangdong Basic and Applied Basic Research Foundation Special Projects——GuangdongShenzhen Joint Funds(2022A1515110027)。
文摘The unprecedented growth of electric vehicles featuring lithium-ion batteries has led to a significant increase in the amount of waste generated,posing pressing waste management challenges for both industry professio nals and environmental regulators.To address these issues,conventio nal pyrometallurgical,hydrometallurgical,and direct recycling methods are commonly employed to promote sustainable battery development.However,these methods are often hindered by laborious purification processes and the generation of low-profit products such as Li_(2)CO_(3),CoSO_(4),NiSO_(4),etc.Herein,an upcycling technology involving a low-temperature solid-to-solid reaction and water leaching procedures is introduced to transform spent LiCoO_(2)cathode materials into value-added cobalt sulfide-based electrocatalysts.The regenerated electrocatalysts exhibit exceptional performance in the oxygen evolution reaction,surpassing that of the benchmark RuO_(2)catalyst.This proposed upcycling method provides researchers with an alternative way to convert the metallic components of waste lithium-ion batteries into high-value Co-,Ni-,Fe-,and Mn-based catalysts.
文摘Poly(ethylene glycol-co-1,4-cyclohexanedimethanol terephthalate)(PETG)possesses excellent properties and stability than traditional poly(ethylene terephthalate)(PET).However,the production and application of PETG are restricted by the expensive monomer(1,4-cyclohexanedimethanol,CHDM).Direct upgrading of waste PET to dimethyl cyclohexane-1,4-dicarboxylate(DMCD)can promote the production of CHDM in large scale.In this work,a bifunctional Ru/UiO-66_(def)-SO_(3)H catalyst was synthesized and utilized in coupled methanolysis(of waste PET to dimethyl terephthalate(DMT))and hydrogenation(of DMT to DMCD)under mild condition.Characterizations revealed that Ru/UiO-66_(def)-SO_(3)H possessed mesopores(dominant channels of 2.72 and 3.44 nm),enlarged surface area(998 m^(2)·g^(–1)),enhanced acidity(580μmol·g^(–1)),and Ru nanoparticles(NPs)dispersed highly(45.1%)compared to those of Ru/UiO-66.These combined advantages could accelerate the methanolysis and hydrogenation reactions simultaneously,promoting the performance of direct upgrading of PET to DMCD in one pot.In particular,the conversion of PET and yield of DMCD over Ru/UiO-66_(def)-SO_(3)H reached 100%and 97.7%at 170℃and 3 MPa H_(2)within 6 h.Moreover,Ru/UiO-66_(def)-SO3H was also capable for the upcycling of waste PET-based products including beverage bottles,textile fiber and packaging film to DMCD.
基金financially supported by the National Natural Science Foundation of China(Nos.52373007 and 52073296)Innovative Leading Talent of Taihu Lake Talent Plan in Wuxi City+1 种基金Zhejiang Ten Thousand Talent ProgramResearch startup fund from Jiangnan University。
文摘Poly(butylene adipate-co-terephthalate)(PBAT),a widely studied biodegradable material,has not effectively addressed the problem of plastic waste.Taking into consideration the cost-effectiveness,upcycling PBAT should take precedence over direct composting degradation.The present work adopts a chain breaking-crosslinking strategy,upcycling PBAT into dual covalent adaptable networks(CANs).During the chainbreaking stage,the ammonolysis between PBAT and polyethyleneimine(PEI)established the primary crosslinked network.Subsequently,styrene maleic anhydride copolymer(SMA)reacted with the hydroxyl group,culminating in the formation of dual covalent adaptable networks.In contrast to PBAT,the PBAT-dual-CANs exhibited a notable Young's modulus of 239 MPa,alongside an inherent resistance to creep and solvents.Owing to catalysis from neighboring carboxyl group and excess hydroxyl groups,the PBAT-dual-CANs exhibited fast stress relaxation.Additionally,they could be recycled through extrusion and hot-press reprocessing,while retaining their biodegradability.This straightforward strategy offers a solution for dealing with plastic waste.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(RS-2023-00302697,2022H1D3A3A01077254)。
文摘Plastic,renowned for its versatility,durability,and cost-effectiveness,is indispensable in modern society.Nevertheless,the annual production of nearly 400 million tons of plastic,coupled with a recycling rate of only 9%,has led to a monumental environmental crisis.Plastic recycling has emerged as a vital response to this crisis,offering sustainable solutions to mitigate its environmental impact.Among these recycling efforts,plastic upcycling has garnered attention,which elevates discarded plastics into higher-value products.Here,electrocatalytic and photoelectrocatalytic treatments stand at the forefront of advanced plastic upcycling.Electrocatalytic or photoelectrocatalytic treatments involve chemical reactions that facilitate electron transfer through the electrode/electrolyte interface,driven by electrical or solar energy,respectively.These methods enable precise control of chemical reactions,harnessing potential,current density,or light to yield valuable chemical products.This review explores recent progress in plastic upcycling through electrocatalytic and photoelectrocatalytic pathways,offering promising solutions to the plastic waste crisis and advancing sustainability in the plastics industry.
基金The Fundamental Research Funds for the Central Universities,HUST,Grant/Award Number:2021GCRC046The Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies,Grant/Award Number:FZ2022005Natural Science Foundation of Hubei Province,China,Grant/Award Number:2022CFA031。
文摘The recycling of spent batteries has become increasingly important owing to their wide applications,abundant raw material supply,and sustainable development.Compared with the degraded cathode,spent anode graphite often has a relatively intact structure with few defects after long cycling.Yet,most spent graphite is simply burned or discarded due to its limited value and inferior performance on using conventional recycling methods that are complex,have low efficiency,and fail in performance restoration.Herein,we propose a fast,efficient,and“intelligent”strategy to regenerate and upcycle spent graphite based on defect‐driven targeted remediation.Using Sn as a nanoscale healant,we used rapid heating(~50 ms)to enable dynamic Sn droplets to automatically nucleate around the surface defects on the graphite upon cooling owing to strong binding to the defects(~5.84 eV/atom),thus simultaneously achieving Sn dispersion and graphite remediation.As a result,the regenerated graphite showed enhanced capacity and cycle stability(458.9 mAh g^(−1) at 0.2 A g^(−1) after 100 cycles),superior to those of commercial graphite.Benefiting from the self‐adaption of Sn dispersion,spent graphite with different degrees of defects can be regenerated to similar structures and performance.EverBatt analysis indicates that targeted regeneration and upcycling have significantly lower energy consumption(~99%reduction)and near‐zero CO_(2) emission,and yield much higher profit than hydrometallurgy,which opens a new avenue for direct upcycling of spend graphite in an efficient,green,and profitable manner for sustainable battery manufacture.
基金supported by the support by the Natural Science Foundation of China projects(Nos.22225604 and 22076082)the Frontiers Science Center for New Organic Matter(No.63181206)Haihe Laboratory of Sustainable Chemical Transformations.
文摘With the rapid development of plastic production and consumption globally,the amount of post-consumer plastic waste has reached levels that have posed environmental threats.Considering the substantial CO_(2)emissions throughout the plastic lifecycle from material production to its disposal,photocatalysis is considered a promising strategy for eff ective plastic recycling and upcycling.It can upgrade plastics into value-added products under mild conditions using solar energy,realizing zero carbon emissions.In this paper,we explain the basics of photocatalytic plastic reformation and underscores plastic feedstock reformation pathways into high-value-added products,including both degradation into CO_(2)followed by reformation and direct reformation into high-value-added products.Finally,the current applications of transforming plastic waste into fuels,chemicals,and carbon materials and the outlook on upcycling plastic waste by photocatalysis are presented,facilitating the realization of carbon neutrality and zero plastic waste.
基金financially supported by the National Key R&D Program of China (2021YFA1501700)the National Science Foundation of China (22272114)+4 种基金the Fundamental Research Funds from Sichuan University (2022SCUNL103)the Funding for Hundred Talent Program of Sichuan University (20822041E4079)the NSFC (22102018 and 52171201)the Huzhou Science and Technology Bureau (2022GZ45)the Hefei National Research Center for Physical Sciences at the Microscale (KF2021005)。
文摘The conversion of waste polylactic acid(PLA)plastics into high-value-added chemicals through electrochemical methods is a promising and sustainable approach.However,developing efficient and highly selective catalysts for lactic acid oxidation reaction(LAOR)and understanding the reaction process are challenging.Here,we report the electrooxidation of waste PLA to acetate at a high current density of 100 mA cm-2 with high Faraday efficiency(~95%)and excellent stability(>100 h)over a nickel selenide nanosheet catalyst.In addition,a total Faraday efficiency of up to 190%was achieved for carboxylic acids,including acetic acid and formic acid,by coupling with the cathodic CO_(2) reduction reaction.In situ experimental results and theoretical simulations revealed that the catalytic activity center of LAOR was dynamically formed NiOOH species,and the surface-adsorbed SeO_(x) species accelerated the formation of Ni~(3+)species,thus promoting catalytic activity.The mechanism of lactic acid electrooxidation was further elucidated.Lactic acid was dehydrogenated to produce pyruvate first and then formed CH_3CO due to preferential C-C bond cleavage,resulting in the presence of acetate.This work demonstrated a sustainable method for recycling waste PLA and CO_(2) into high-value-added products.
基金supported by the National Natural Science Foundation of China(52373099)the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)。
文摘The integration of interfacial solar steam generation and photocatalytic degradation technology has pro-vided a promising platform to simultaneously produce freshwater and degrade pollutants.However,con-structing low-cost,multi-functional evaporators for treating Cr(Ⅵ)-polluted water remains challenging,and the synergistic mechanism on Cr(Ⅵ)reduction is fuzzy.Herein,we propose the combined strategy of ball milling and solution mixing for the sustainable production of Bi-MOF microrod from waste poly(ethylene terephthalate),and construct Bi-MOF-based solar evaporators for simultaneous photo-Fenton Cr(Ⅵ)reduction and freshwater production.Firstly,the evaporator comprised of Bi-MOF microrod and graphene nanosheet possesses high light absorption,efficient photothermal conversion,and good hydro-philic property.Attributing to the advantages,the hybrid evaporator exhibits the evaporation rate of 2.16 kg m^(-2) h^(-1) and evaporation efficiency of 87.5%under 1 kW m^(-2) of irradiation.When integrating with photo-Fenton reaction,the Cr(Ⅵ)reduction efficiency is 91.3%,along with the reaction kinetics of 0.0548 min^(-1),surpassing many advanced catalysts.In the outdoor freshwater production and Cr(Ⅵ)reduction,the daily accumulative water yield is 5.17 kg m^(-2) h^(-1),and the Cr(Ⅵ)reduction efficiency is 99.9%.Furthermore,we prove that the localization effect derived from the interfacial solar-driven evap-oration enhances H_(2)O_(2) activation for the photo-Fenton reduction of Cr(Ⅵ).Based on the result of density functional theory,Bi-MOF microrod provides rich active centers for H_(2)O_(2) activation to produce active sites such as e-or-O_(2).This study not only proposes a new strategy to construct multi-functional solar evaporators for freshwater production and catalytic reduction of pollutants,but also advances the chem-ical upcycling of waste polyesters.
基金supported by the National Natural Science Foundation of China(52276202)the Tsinghua-Toyota Joint Research Fund.
文摘As global municipal solid waste(MSW)quantities continue to escalate,serious socio-environmental challenges arise,necessitating innovative solutions.Waste-to-hydrogen(WTH)via two-stage gasification-reforming(TSGR)presents an emergent technology for MSW upcycling,offering to ease waste management burdens and bolster the burgeoning hydrogen economy.Despite early initiatives to advance TSGR technology,a cohesive and critical analysis of cutting-edge knowledge and strategies to enhance hydrogen production remains lacking.This review aggregates literature on MSW upcycling to hydrogen via TSGR,with a focus on optimizing process control and catalytic efficiency.It underscores technological avenues to augment hydrogen output,curtail catalyst costs,and refine system performance.Particularly,the review illuminates the potential for integrating chemical and calcium looping into TSGR processes,identifying opportunities,and pinpointing challenges.The review concludes with a summary of the current state of techno-economic analysis for this technology,presenting outstanding challenges and future research directions,with the ultimate goal of transitioning WTH from theoretical to practical application.
