Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fund...Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fundamental trade-off between haze and transparency,coupled with impractical thicknesses(≥1 mm).Inspired by squid’s skin-peeling mechanism,this work develops a peroxyformic acid(HCOOOH)-enabled precision peeling strategy to isolate intact 10-μm-thick bamboo green(BG)frameworks—100×thinner than wood-based counterparts while achieving an unprecedented optical performance(88%haze with 80%transparency).This performance surpasses delignified biomass(transparency<40%at 1 mm)and matches engineered cellulose composites,yet requires no energy-intensive nanofibrillation.The preserved native cellulose I crystalline structure(64.76%crystallinity)and wax-coated uniaxial fibril alignment(Hermans factor:0.23)contribute to high mechanical strength(903 MPa modulus)and broadband light scattering.As a light-management layer in polycrystalline silicon solar cells,the BG framework boosts photoelectric conversion efficiency by 0.41%absolute(18.74%→19.15%),outperforming synthetic anti-reflective coatings.The work establishes a scalable,waste-to-wealth route for optical-grade cellulose materials in next-generation optoelectronics.展开更多
Hydrothermal treatment of cellulose is a promising green route for bioenergy and biochemical production,yet it requires investigation of the underlying mechanisms.In this study,the effects of cellulose crystallinity a...Hydrothermal treatment of cellulose is a promising green route for bioenergy and biochemical production,yet it requires investigation of the underlying mechanisms.In this study,the effects of cellulose crystallinity and decoupled temperature and pressure conditions on cellulose conversion and product distribution were investigated.Microcrystalline cellulose was ball-milled for varying durations,leading to a reduction in crystallinity,with 4 h of milling sufficient to achieve near-complete amorphization.Unlike concurrent recrystallization and hydrolysis observed under autogenous pressure,decoupled conditions significantly accelerated hydrolysis of cellulose.Notably,lower crystallinity cellulose exhibited significant improvements in glucose and 5-HMF yields,with 4-h ball milling showing optimal performance among all samples.Furthermore,carbon sub-micron spheres were largely produced,which were confirmed via PTFE encapsulation experiments to primarily consist of secondary char deriving from re-polymerization and condensation reactions of the liquid phase.Overall,this study demonstrates that lower crystallinity not only facilitates hydrolysis but also accelerates the carbonization processes under decoupled pressure conditions,highlighting its potential for efficient biomass conversion into valuable products.展开更多
The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their l...The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their low gravimetric energy density(approximately 35 Wh kg^(-1)),far below lithium-ion batteries(exceeding 200 Wh kg^(-1)),and a limited operational temperature range(from-20℃ to 60℃),restricting their use in extreme environments.To date,no comprehensive review has elucidated the crucial role of the chemistry and structure-property relationships of CBMs in advancing FSC technology.This review fills this gap by examining the chemical attributes and versatility of cellulose and its derivatives,including their physicochemical characteris-tics,assembly methodologies,and functional modifications such as oxidation,esterification,etherification,grafting polymerization,nucleophilic substitution,and crosslinking reactions.We further provide an overview of the chemistry and structure-function correlations of various cellulose forms used in advanced electrodes,solid electrolytes,separators,binders,current collectors,and substrate/encapsulation materials,alongside relevant microelectrode processing technologies.Given that large-scale application of FSCs is still in its early stages,we offer insightful design principles for guiding future development of cellulose-based FSCs.By proposing a“chemistry-performance-sustainability”design framework,this review not only addresses existing limitations but also outlines a roadmap for next-generation eco-friendly FSCs.展开更多
Cellulose,the most abundant and renewable biopolymer,offers a sustainable and cost-effective solution for regulating lithium electrodeposition toward safer lithium metal batteries,thanks to its high nanofibrous struct...Cellulose,the most abundant and renewable biopolymer,offers a sustainable and cost-effective solution for regulating lithium electrodeposition toward safer lithium metal batteries,thanks to its high nanofibrous structure and intrinsic lithiophilic property.In this work,we introduce interface-engineered cellulose-based separators by converting intrinsic hydroxyl groups on cellulose nanofibers(CNFs)to nitrogen functionalities through a trace conducting polymer coating.Both experimental and theoretical results reveal that the nitrogen moieties disrupt the compact hydrogen bond network within hydroxyl cellulose,enabling multiple nitrogen-lithium interactions that enhance lithium ion transport.In addition to an extraordinary Li^(+)transference number of 0.86 and a high ionic conductivity of 1.1 mS cm^(-1),the nitrogen-functionalized CNF contributes to a uniform electric field and Li^(+)concentration distribution across the lithium metal surface.This facilitates the formation of a LiF-rich solid electrolyte interface and suppresses Li dendrite growth.Consequently,Li‖Li cells demonstrate stable plating/stripping cycles for approximately 3000 h at a current density of 1 mA cm^(-2) with a fixed capacity of 1 mAh cm^(-2),while maintaining a low overpotential of 15 mV.Our work provides valuable insights into the surface functionalization of natural biomass for advancing sustainable energy storage technologies.展开更多
The valorization of agricultural waste into high-value nanomaterials is crucial for advancing sustainable biorefineries.This study presents an efficient approach for extracting carboxylated cellulose nanocrystals(CNCs...The valorization of agricultural waste into high-value nanomaterials is crucial for advancing sustainable biorefineries.This study presents an efficient approach for extracting carboxylated cellulose nanocrystals(CNCs)from poplar leaf waste(PL),an abundant and underutilized biomass.The process involved alkaline treatment and hydrogen peroxide bleaching to purify cellulose(PL-CEL),followed by sequential periodate-chlorite oxidation to produce dicarboxylic cellulose nanocrystals(PL-CNCs).The resulting nanocrystals were comprehensively characterized using compositional analysis,XRD,FTIR,TEM,TGA,and zeta potential measurements.XRD analysis confirmed a high crystallinity index of 82%for PL-CEL,which decreased to 72.2%after oxidation due to the introduction of carboxyl groups.FTIR spectra revealed a prominent peak at 1720 cm-1,confirming successful carboxylation.TEM images showed rod-like nanocrystalswith an average length of 271.22 nmand width of 14.68 nm,while conductometric titration indicated a carboxyl content of 1.9 mmol/g.The PL-CNCs exhibited good colloidal stability with a zeta potential of-30.2mV at pH7.0.TGA demonstratedmoderate thermal stability with enhanced char formation.This work highlights a green and scalable route for converting poplar leaf waste into functional nanocellulose,suitable for applications in composites,adsorption,and sustainable materials.The novelty of this study lies in the pioneering use of poplar leaf waste combined with a sequential periodate-chlorite oxidation to sustainably produce carboxylated CNCs with enhanced functionality.展开更多
基金supported by National Natural Science Foundation of China(32494793).
文摘Cellulose frameworks have emerged as promising materials for light management due to their exceptional light-scattering capabilities and sustainable nature.Conventional biomass-derived cellulose frameworks face a fundamental trade-off between haze and transparency,coupled with impractical thicknesses(≥1 mm).Inspired by squid’s skin-peeling mechanism,this work develops a peroxyformic acid(HCOOOH)-enabled precision peeling strategy to isolate intact 10-μm-thick bamboo green(BG)frameworks—100×thinner than wood-based counterparts while achieving an unprecedented optical performance(88%haze with 80%transparency).This performance surpasses delignified biomass(transparency<40%at 1 mm)and matches engineered cellulose composites,yet requires no energy-intensive nanofibrillation.The preserved native cellulose I crystalline structure(64.76%crystallinity)and wax-coated uniaxial fibril alignment(Hermans factor:0.23)contribute to high mechanical strength(903 MPa modulus)and broadband light scattering.As a light-management layer in polycrystalline silicon solar cells,the BG framework boosts photoelectric conversion efficiency by 0.41%absolute(18.74%→19.15%),outperforming synthetic anti-reflective coatings.The work establishes a scalable,waste-to-wealth route for optical-grade cellulose materials in next-generation optoelectronics.
基金The financial support from the Beijing Natural Science Foundation(JQ24053)National Natural Science Foundation of China(52276202)+3 种基金Natural Science Foundation of Shanxi Province(202403021211024,202403021212148)Yunnan Major Scientific and Technological Projects(202302AQ370003)Huaneng Group Science and Technology Research Project(HNKJ23-H71)Tsinghua University Initiative Scientific Research Program are gratefully acknowledged.
文摘Hydrothermal treatment of cellulose is a promising green route for bioenergy and biochemical production,yet it requires investigation of the underlying mechanisms.In this study,the effects of cellulose crystallinity and decoupled temperature and pressure conditions on cellulose conversion and product distribution were investigated.Microcrystalline cellulose was ball-milled for varying durations,leading to a reduction in crystallinity,with 4 h of milling sufficient to achieve near-complete amorphization.Unlike concurrent recrystallization and hydrolysis observed under autogenous pressure,decoupled conditions significantly accelerated hydrolysis of cellulose.Notably,lower crystallinity cellulose exhibited significant improvements in glucose and 5-HMF yields,with 4-h ball milling showing optimal performance among all samples.Furthermore,carbon sub-micron spheres were largely produced,which were confirmed via PTFE encapsulation experiments to primarily consist of secondary char deriving from re-polymerization and condensation reactions of the liquid phase.Overall,this study demonstrates that lower crystallinity not only facilitates hydrolysis but also accelerates the carbonization processes under decoupled pressure conditions,highlighting its potential for efficient biomass conversion into valuable products.
基金support from the National Key R&D Program of China(Grant No.2023YFB4005204)the National Natural Science Foundation of China(Grant No.22125903,U24A20553,22579025,52502038)+2 种基金Fundamental Research Funds for the Central Universities(No.2572023CT06)Key Joint Project of the Natural Science Foundation of Heilongjiang Province,China(No.ZL2024E007)the Innovation Foundation for Doctoral Program of Forestry Engineering of Northeast Forestry University(No.LYGC202220).
文摘The demand for sustainable energy storage has accelerated the development of cellulose-based materials(CBMs)for flexible supercapacitors(FSCs).However,widespread commercialization of FSCs remains challenged by their low gravimetric energy density(approximately 35 Wh kg^(-1)),far below lithium-ion batteries(exceeding 200 Wh kg^(-1)),and a limited operational temperature range(from-20℃ to 60℃),restricting their use in extreme environments.To date,no comprehensive review has elucidated the crucial role of the chemistry and structure-property relationships of CBMs in advancing FSC technology.This review fills this gap by examining the chemical attributes and versatility of cellulose and its derivatives,including their physicochemical characteris-tics,assembly methodologies,and functional modifications such as oxidation,esterification,etherification,grafting polymerization,nucleophilic substitution,and crosslinking reactions.We further provide an overview of the chemistry and structure-function correlations of various cellulose forms used in advanced electrodes,solid electrolytes,separators,binders,current collectors,and substrate/encapsulation materials,alongside relevant microelectrode processing technologies.Given that large-scale application of FSCs is still in its early stages,we offer insightful design principles for guiding future development of cellulose-based FSCs.By proposing a“chemistry-performance-sustainability”design framework,this review not only addresses existing limitations but also outlines a roadmap for next-generation eco-friendly FSCs.
基金supported by the National Natural Science Foundation of China(Grant No.22479046,22461142135)。
文摘Cellulose,the most abundant and renewable biopolymer,offers a sustainable and cost-effective solution for regulating lithium electrodeposition toward safer lithium metal batteries,thanks to its high nanofibrous structure and intrinsic lithiophilic property.In this work,we introduce interface-engineered cellulose-based separators by converting intrinsic hydroxyl groups on cellulose nanofibers(CNFs)to nitrogen functionalities through a trace conducting polymer coating.Both experimental and theoretical results reveal that the nitrogen moieties disrupt the compact hydrogen bond network within hydroxyl cellulose,enabling multiple nitrogen-lithium interactions that enhance lithium ion transport.In addition to an extraordinary Li^(+)transference number of 0.86 and a high ionic conductivity of 1.1 mS cm^(-1),the nitrogen-functionalized CNF contributes to a uniform electric field and Li^(+)concentration distribution across the lithium metal surface.This facilitates the formation of a LiF-rich solid electrolyte interface and suppresses Li dendrite growth.Consequently,Li‖Li cells demonstrate stable plating/stripping cycles for approximately 3000 h at a current density of 1 mA cm^(-2) with a fixed capacity of 1 mAh cm^(-2),while maintaining a low overpotential of 15 mV.Our work provides valuable insights into the surface functionalization of natural biomass for advancing sustainable energy storage technologies.
基金funded by the basic scientific research Funds project of Heilongjiang Universities,grant number 2023-KYYWF-0570.
文摘The valorization of agricultural waste into high-value nanomaterials is crucial for advancing sustainable biorefineries.This study presents an efficient approach for extracting carboxylated cellulose nanocrystals(CNCs)from poplar leaf waste(PL),an abundant and underutilized biomass.The process involved alkaline treatment and hydrogen peroxide bleaching to purify cellulose(PL-CEL),followed by sequential periodate-chlorite oxidation to produce dicarboxylic cellulose nanocrystals(PL-CNCs).The resulting nanocrystals were comprehensively characterized using compositional analysis,XRD,FTIR,TEM,TGA,and zeta potential measurements.XRD analysis confirmed a high crystallinity index of 82%for PL-CEL,which decreased to 72.2%after oxidation due to the introduction of carboxyl groups.FTIR spectra revealed a prominent peak at 1720 cm-1,confirming successful carboxylation.TEM images showed rod-like nanocrystalswith an average length of 271.22 nmand width of 14.68 nm,while conductometric titration indicated a carboxyl content of 1.9 mmol/g.The PL-CNCs exhibited good colloidal stability with a zeta potential of-30.2mV at pH7.0.TGA demonstratedmoderate thermal stability with enhanced char formation.This work highlights a green and scalable route for converting poplar leaf waste into functional nanocellulose,suitable for applications in composites,adsorption,and sustainable materials.The novelty of this study lies in the pioneering use of poplar leaf waste combined with a sequential periodate-chlorite oxidation to sustainably produce carboxylated CNCs with enhanced functionality.
