LiMn_(2)O_(4)(LMO)electrochemical lithium-ion pump has gained widespread attention due to its green,high efficiency,and low energy consumption in selectively extracting lithium from brine.However,collapse of crystal s...LiMn_(2)O_(4)(LMO)electrochemical lithium-ion pump has gained widespread attention due to its green,high efficiency,and low energy consumption in selectively extracting lithium from brine.However,collapse of crystal structure and loss of lithium extraction capacity caused by Mn dissolution loss limits its industrialized application.Hence,a multifunctional coating was developed by depositing amorphous AlPO_(4)on the surface of LMO using sol-gel method.The characterization and electrochemical performance test provided insights into the mechanism of Li^(+)embedment and de-embedment and revealed that multifunctional AlPO_(4)can reconstruct the physical and chemical state of LMO surface to improve the interface hydrophilicity,promote the transport of Li^(+),strengthen cycle stability.Remarkably,after 20 cycles,the capacity retention rate of 0.5AP-LMO reached 93.6%with only 0.147%Mn dissolution loss.The average Li^(+)release capacity of 0.5AP-LMO//Ag system in simulated brine is 28.77 mg/(g h),which is 90.4%higher than LMO.Encouragingly,even in the more complex Zabuye real brine,0.5AP-LMO//Ag can still maintain excellent lithium extraction performance.These results indicate that the 0.5AP-LMO//Ag lithium-ion pump shows promising potential as a Li^(+)selective extraction system.展开更多
A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structur...A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.展开更多
Accelerating the development of lithium resources has attracted a great deal of attention with the explosive growth of new energy vehicles.As a new technology,electrochemical lithium ion pumping(ELIP)is featured by en...Accelerating the development of lithium resources has attracted a great deal of attention with the explosive growth of new energy vehicles.As a new technology,electrochemical lithium ion pumping(ELIP)is featured by environment-friendly,low energy consumption and high efficiency.This review summarizes the research progress in ELIP,and focuses on the evaluation methods,electrode materials and electrochemical systems of ELIP.It can be concluded that ELIP is expected to achieve an industrial application and has a promising prospect.In addition,challenges and perspective of electrochemical lithium extraction are also highlighted.展开更多
Poly-3-hydroxybutyrate （PHB） can be produced by various species of bacteria. Among the possible carbon sources, both methane and methanol could be a suitable substrate for the production of PHB. Methane is cheap and...Poly-3-hydroxybutyrate （PHB） can be produced by various species of bacteria. Among the possible carbon sources, both methane and methanol could be a suitable substrate for the production of PHB. Methane is cheap and plentiful not only as natural gas, but also as biogas. Methanol can also maintain methanotrophic activity in some conditions. The methanotrophic strain Methylosinus trichosporium IMV3011 can accumulate PHB with methane and methanol in a brief nonsterile process. Liquid methanol （0.1%） was added to improve the oxidization of methane. The studies were carried out using shake flasks. Cultivation was performed in two stages： a continuous growth phase and a PHB accumulation phase under the conditions short of essential nutrients （ammonium, nitrate, phosphorus, copper, iron （Ⅲ）, magnesium or ethylenediamine tetraacetate （EDTA）） in batch culture. It was found that the most suitable growth time for the cell is 144 h. Then an optimized culture condition for second stage was determined, in which the PHB concentration could be much increased to 0.6 g/L. In order to increase PHB content, citric acid was added as an inhibitor of tricarboxylic acid cycle （TCA）. It was found that citric acid is favorable for the PHB accumulation, and the PHB yield was increased to 40% （w/w） from the initial yield of 12% （w/w） after nutrient deficiency cultivation. The PHB produced is of very high quality with molecular weight up to 1.5 × 10^6Da.展开更多
The rapid commercialization of lithium–ion batteries has caused significant expansion of the lithium demand.Electrochemical lithium ions pump is a promising technology because of its good selectivity and friendly env...The rapid commercialization of lithium–ion batteries has caused significant expansion of the lithium demand.Electrochemical lithium ions pump is a promising technology because of its good selectivity and friendly environment.Herein,an Al_(2)O_(3)–ZrO_(2) film coating of the LiMn_(2)O_(4)(AlZr–LMO) electrode is prepared and operated for recovery of Li^(+)from brine.The Li^(+) maximum extraction capacity of AlZr–LMO reached 49.92 mg/g in one cycle.Compared with the solely LMO electrode,the AlZr–LMO demonstrated evident electrochemical stability and cycle life towards the Li^(+)recovery system.After 30 successive cycles,the extraction capacity for Li^(+)increased from 29.21%to 57.67%.The high cycle capacity of the material could be attributed to its low polarization,high active sites,and good chemical stability of the electrode surface owing to the synergy function of Al_(2)O_(3)–ZrO_(2)in the charging-discharging process.A dynamic model parameter identification method was performed to evaluate the active site of AlZr–LMO.This work may provide a way to design the AlZr–LMO electrode and develop a good method for the recovery of lithium from brine.展开更多
Oxidative desulfurization(ODS)has been proved to be an efficient strategy for the production of clean fuel oil.Numerous metal-based materials have been employed as excellent ODS catalysts,but being hindered by their h...Oxidative desulfurization(ODS)has been proved to be an efficient strategy for the production of clean fuel oil.Numerous metal-based materials have been employed as excellent ODS catalysts,but being hindered by their high-cost and potential secondary pollution.In this work,we employed graphene analogous hexagonal boron nitride(h-BN)as a metal-free catalyst for ODS with hydrogen peroxide(H2O2)as the oxidant.The h-BN catalyst was characterized and proved to be a few-layered structure with relatively high specific surface areas.The h-BN catalyst showed a 99.4%of sulfur removal in fuel oil under the optimized reaction conditions.Besides,the h-BN can be recycled for 8 times without significant decrease in the catalytic performance.Detailed mechanism analysis found that it is the boron radicals in h-BN activated H2O2 to generate·OH species,which can readily oxidize sulfides to corresponding sulfones for separation.This work would provide another choice in choosing metal-free catalysts for ODS.展开更多
Construction of catalysts with integral structure for oxidative reaction process is an essential promotion to catalysts in industrial application.In this work,a 3D printing method was employed to prepare 3D printed sp...Construction of catalysts with integral structure for oxidative reaction process is an essential promotion to catalysts in industrial application.In this work,a 3D printing method was employed to prepare 3D printed spheres(3D-PSs),followed by carbonization to form 3D carbon spheres(3D-CSs).Then,a 3D-CSs supported phosphotungstic acid(HPW/3D-CSs)was prepared for deep oxidative desulfurization.Compared with traditional powder catalysts,the as-prepared catalyst is easy to be operated and separated from oil products.The supported catalyst possesses excellent catalytic performance and the removal of DBT,4-MDBT and 4,6-DMDBT in fuel oil,reaching^100%of sulfur removal.The effects of various experimental parameters on desulfurization efficiency were considered to optimize reaction conditions.Moreover,the catalyst shows excellent thermal and chemical stability,with no obvious decrease in desulfurization activity after 5 cycles.GC–MS analysis indicates DBT sulfone was the solely oxidized product of DBT.展开更多
In recent years, transition-metal oxides(TMOs) have been long employed for aerobic oxidative desulfurization. However, the inherent bottlenecks, such as the low explosion of active sites, limit the application of bulk...In recent years, transition-metal oxides(TMOs) have been long employed for aerobic oxidative desulfurization. However, the inherent bottlenecks, such as the low explosion of active sites, limit the application of bulk TMOs catalyst. In this study, V_(2)O_(5) nanoparticles with oxygen vacancies were prepared in large-scale via facile ball milling strategy with adding oxalic acid as a reducing agent. The as-prepared catalysts exhibit remarkable sulfur removal for oils with different initial S-concentrations and different substrates. Sulfur removal could reach up to 99.7%(< 2 ppm) under the optimized reaction conditions. This work provides a feasible desulfurization strategy for fuel oils.展开更多
The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery s...The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.展开更多
Non-noble metal-based catalysts,especially stable ones,have gained increasing attentions in the field of electronically catalytic hydrogen evolution reaction(HER).In this work,an N-doped carbon confined Co–Ni alloy w...Non-noble metal-based catalysts,especially stable ones,have gained increasing attentions in the field of electronically catalytic hydrogen evolution reaction(HER).In this work,an N-doped carbon confined Co–Ni alloy with reduced graphene oxide(rGO) decoration(CoNi@N-C/rGO) was fabricated for HER.The prepared catalyst exhibited excellent HER activity in an acidic electrolyte(Tafel slope of ～133.7 m V).The results showed that the enhanced HER performance of the nanostructures is attributed to the chemical and electronic synergic effect between the confined Co–Ni alloy and r GO.Stability tests,realized via longterm potential cycles and extended electrolysis,provided the confirmation of the exceptional durability of the catalyst,which originated from the confining effect of the N-doped carbon shell.This versatile method provides a strategy for designing stable non-precious metal electrocatalysts confined by carboncoating.展开更多
High-quality graphene flakes have long been desirable for numerous applications including energy stor- age, printable electronics, and catalysis. In this contribution, we report a green, efficient, facile gas-driven e...High-quality graphene flakes have long been desirable for numerous applications including energy stor- age, printable electronics, and catalysis. In this contribution, we report a green, efficient, facile gas-driven exfoliation process for the preparation of high-quality graphene in large scale. The gas exfoliation process was realized by the interplay between the expansion of interlayer at high temperature and the gasifi- cation of liquid nitrogen within the interlayer. Detailed experiments demonstrated that the higher tem- perature was critical to the formation of fewer layers. The exfoliated graphene was proved to be of high quality. We further investigated the electrochemical behavior of this exfoliated graphene. As a result, this few-layered graphene demonstrated an enhanced capability as a supercapacitor, much higher than its counterpart parent material.展开更多
基金supported by the National Natural Science Foundation of China(21908082,22278426,and 22178154)the Jiangsu Funding Program for Excellent Postdoctoral Talent(2022ZB629)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20221367)the China Postdoctoral Science Foundation(2021M701472)。
文摘LiMn_(2)O_(4)(LMO)electrochemical lithium-ion pump has gained widespread attention due to its green,high efficiency,and low energy consumption in selectively extracting lithium from brine.However,collapse of crystal structure and loss of lithium extraction capacity caused by Mn dissolution loss limits its industrialized application.Hence,a multifunctional coating was developed by depositing amorphous AlPO_(4)on the surface of LMO using sol-gel method.The characterization and electrochemical performance test provided insights into the mechanism of Li^(+)embedment and de-embedment and revealed that multifunctional AlPO_(4)can reconstruct the physical and chemical state of LMO surface to improve the interface hydrophilicity,promote the transport of Li^(+),strengthen cycle stability.Remarkably,after 20 cycles,the capacity retention rate of 0.5AP-LMO reached 93.6%with only 0.147%Mn dissolution loss.The average Li^(+)release capacity of 0.5AP-LMO//Ag system in simulated brine is 28.77 mg/(g h),which is 90.4%higher than LMO.Encouragingly,even in the more complex Zabuye real brine,0.5AP-LMO//Ag can still maintain excellent lithium extraction performance.These results indicate that the 0.5AP-LMO//Ag lithium-ion pump shows promising potential as a Li^(+)selective extraction system.
基金financial support from the National Natural Science Foundation of China(22178154,22008094,21908082,21878133)Natural Science Foundation of Jiangsu Province(BK20190852,BK20190854)Natural Science Foundation for Jiangsu Colleges and Universities(19KJB530005).
文摘A few-layered hexagonal boron nitride nanosheets stabilized platinum nanoparticles(Pt/h-BNNS)is engineered for oxidation-promoted adsorptive desulfurization(OPADS)of fuel oil.It was found that the few-layered structure and the defective sites of h-BNNS not only are beneficial to the stabilization of Pt NPs but also favor the adsorption of aromatic sulfides.By employing Pt/h-BNNS with a Pt loading amount of 1.19 wt%as the active adsorbent and air as an oxidant,a 98.0%sulfur removal over dibenzothiophene(DBT)is achieved along with a total conversion of the DBT to the corresponding sulfones(DBTO_(2)).Detailed experiments show that the excellent desulfurization activity originates from the few-layered structure of h-BNNS and the high catalytic activity of Pt NPs.In addition,the OPADS system with Pt/h-BNNS as the active adsorbent shows remarkable stability in desulfurization performance with the existence of different interferents such as olefin,and aromatic hydrocarbons.Besides,the Pt/h-BNNS can be recycled 12 times without a significant decrease in desulfurization performance.Also,a process flow diagram is proposed for deep desulfurization of fuel oil and recovery of high value-added products,which would promote the industrial application of such OPADS strategy.
基金supported by the National Natural Science Foundation of China(grant numbers 21878133,21908082 and 21722604)the Natural Science Foundation of Jiangsu Province(BK20190854)+2 种基金the China Postdoctoral Science Foundation(2020M671364)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX191622)the Science&Technology Foundation of Zhenjiang(GY2020027)。
文摘Accelerating the development of lithium resources has attracted a great deal of attention with the explosive growth of new energy vehicles.As a new technology,electrochemical lithium ion pumping(ELIP)is featured by environment-friendly,low energy consumption and high efficiency.This review summarizes the research progress in ELIP,and focuses on the evaluation methods,electrode materials and electrochemical systems of ELIP.It can be concluded that ELIP is expected to achieve an industrial application and has a promising prospect.In addition,challenges and perspective of electrochemical lithium extraction are also highlighted.
基金New Century Excellent Talents in University of China(NCET-05-0358)the National Natural Science Foundation of China(20625308)
文摘Poly-3-hydroxybutyrate （PHB） can be produced by various species of bacteria. Among the possible carbon sources, both methane and methanol could be a suitable substrate for the production of PHB. Methane is cheap and plentiful not only as natural gas, but also as biogas. Methanol can also maintain methanotrophic activity in some conditions. The methanotrophic strain Methylosinus trichosporium IMV3011 can accumulate PHB with methane and methanol in a brief nonsterile process. Liquid methanol （0.1%） was added to improve the oxidization of methane. The studies were carried out using shake flasks. Cultivation was performed in two stages： a continuous growth phase and a PHB accumulation phase under the conditions short of essential nutrients （ammonium, nitrate, phosphorus, copper, iron （Ⅲ）, magnesium or ethylenediamine tetraacetate （EDTA）） in batch culture. It was found that the most suitable growth time for the cell is 144 h. Then an optimized culture condition for second stage was determined, in which the PHB concentration could be much increased to 0.6 g/L. In order to increase PHB content, citric acid was added as an inhibitor of tricarboxylic acid cycle （TCA）. It was found that citric acid is favorable for the PHB accumulation, and the PHB yield was increased to 40% （w/w） from the initial yield of 12% （w/w） after nutrient deficiency cultivation. The PHB produced is of very high quality with molecular weight up to 1.5 × 10^6Da.
基金supported by the National Natural Science Foundation of China (21878133, 21908082, 22178154)the Natural Science Foundation of Jiangsu Province (BK20190854)+1 种基金the China Postdoctoral Science Foundation (2020M671364, 2021M701472)the Science & Technology Foundation of Zhenjiang (GY2020027)。
文摘The rapid commercialization of lithium–ion batteries has caused significant expansion of the lithium demand.Electrochemical lithium ions pump is a promising technology because of its good selectivity and friendly environment.Herein,an Al_(2)O_(3)–ZrO_(2) film coating of the LiMn_(2)O_(4)(AlZr–LMO) electrode is prepared and operated for recovery of Li^(+)from brine.The Li^(+) maximum extraction capacity of AlZr–LMO reached 49.92 mg/g in one cycle.Compared with the solely LMO electrode,the AlZr–LMO demonstrated evident electrochemical stability and cycle life towards the Li^(+)recovery system.After 30 successive cycles,the extraction capacity for Li^(+)increased from 29.21%to 57.67%.The high cycle capacity of the material could be attributed to its low polarization,high active sites,and good chemical stability of the electrode surface owing to the synergy function of Al_(2)O_(3)–ZrO_(2)in the charging-discharging process.A dynamic model parameter identification method was performed to evaluate the active site of AlZr–LMO.This work may provide a way to design the AlZr–LMO electrode and develop a good method for the recovery of lithium from brine.
基金All authors appreciate the financial support from the National Key R&D Program of China(2017YFB0306504)the National Natural Science Foundation of China(No.21722604,21878133 and 21908082)+2 种基金China Postdoctoral Science Foundation(No.2019M651743)Natural Science Foundation of Jiangsu Province(BK20190852,BK20190854)Natural Science Foundation for Jiangsu Colleges and Universities(19KJB530005).
文摘Oxidative desulfurization(ODS)has been proved to be an efficient strategy for the production of clean fuel oil.Numerous metal-based materials have been employed as excellent ODS catalysts,but being hindered by their high-cost and potential secondary pollution.In this work,we employed graphene analogous hexagonal boron nitride(h-BN)as a metal-free catalyst for ODS with hydrogen peroxide(H2O2)as the oxidant.The h-BN catalyst was characterized and proved to be a few-layered structure with relatively high specific surface areas.The h-BN catalyst showed a 99.4%of sulfur removal in fuel oil under the optimized reaction conditions.Besides,the h-BN can be recycled for 8 times without significant decrease in the catalytic performance.Detailed mechanism analysis found that it is the boron radicals in h-BN activated H2O2 to generate·OH species,which can readily oxidize sulfides to corresponding sulfones for separation.This work would provide another choice in choosing metal-free catalysts for ODS.
基金financially supported by the National Natural Science Foundation of China(Nos.21722604,21576122,21878133)China Postdoctoral Science Foundation(No.2019M651743)。
文摘Construction of catalysts with integral structure for oxidative reaction process is an essential promotion to catalysts in industrial application.In this work,a 3D printing method was employed to prepare 3D printed spheres(3D-PSs),followed by carbonization to form 3D carbon spheres(3D-CSs).Then,a 3D-CSs supported phosphotungstic acid(HPW/3D-CSs)was prepared for deep oxidative desulfurization.Compared with traditional powder catalysts,the as-prepared catalyst is easy to be operated and separated from oil products.The supported catalyst possesses excellent catalytic performance and the removal of DBT,4-MDBT and 4,6-DMDBT in fuel oil,reaching^100%of sulfur removal.The effects of various experimental parameters on desulfurization efficiency were considered to optimize reaction conditions.Moreover,the catalyst shows excellent thermal and chemical stability,with no obvious decrease in desulfurization activity after 5 cycles.GC–MS analysis indicates DBT sulfone was the solely oxidized product of DBT.
基金financial support from the National Natural Science Foundation of China(21722604)China Postdoctoral Science Foundation(2020M671364,2020M671365)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20190243)the Qinglan Project of Jiangsu Province,and the Society Development Fund of Zhenjiang(SH2020020)。
文摘In recent years, transition-metal oxides(TMOs) have been long employed for aerobic oxidative desulfurization. However, the inherent bottlenecks, such as the low explosion of active sites, limit the application of bulk TMOs catalyst. In this study, V_(2)O_(5) nanoparticles with oxygen vacancies were prepared in large-scale via facile ball milling strategy with adding oxalic acid as a reducing agent. The as-prepared catalysts exhibit remarkable sulfur removal for oils with different initial S-concentrations and different substrates. Sulfur removal could reach up to 99.7%(< 2 ppm) under the optimized reaction conditions. This work provides a feasible desulfurization strategy for fuel oils.
基金supported by the National Natural Science Foundation of China (21878133,21908082,22178154)the Natural Science Foundation of Jiangsu Province(BK20190854)+1 种基金the China Postdoctoral Science Foundation(2020M671364,2021M701472)the Science&Technology Foundation of Zhenjiang (GY2020027)。
文摘The extraction of lithium from salt lakes or seawater has attracted worldwide attention because of the explosive growth of global demand for lithium products. The LiMn_(2)O_(4)-based electrochemical lithium recovery system is one of the strongest candidates for commercial application due to its high inserted capacity and low energy consumption. However, the surface orientation of LiMn_(2)O_(4)that facilitates Li diffusion happens to be prone to manganese dissolution making it a great challenge to obtain high lithium inserted capacity and long life simultaneously. Herein, we address this problem by designing a truncated octahedral LiMn_(2)O_(4)(Tr-oh LMO) in which the dominant(111) facets minimize Mn dissolution while a small portion of(100) facets facilitate the Li diffusion. Thus, this Tr-oh LMO-based electrochemical lithium recovery system shows excellent Li recovery performance with high inserted capacity(20.25 mg g^(-1)per cycle) in simulated brine. In addition, the dissolution rate of manganese per 30 cycles is only 0.44% and the capacity maintained 85% of the initial after 30 cycles. These promising findings accelerate the practical application of LiMn_(2)O_(4)in electrochemical lithium recovery.
基金financial support from the National Natural Science Foundation (21676129,21607063)the Science & Technology Foundation of Zhenjiang (GY2016021,GY2017001,GY2017009)Postgraduate Innovation Project of Jiangsu Province (KYLX16_0912)
文摘Non-noble metal-based catalysts,especially stable ones,have gained increasing attentions in the field of electronically catalytic hydrogen evolution reaction(HER).In this work,an N-doped carbon confined Co–Ni alloy with reduced graphene oxide(rGO) decoration(CoNi@N-C/rGO) was fabricated for HER.The prepared catalyst exhibited excellent HER activity in an acidic electrolyte(Tafel slope of ～133.7 m V).The results showed that the enhanced HER performance of the nanostructures is attributed to the chemical and electronic synergic effect between the confined Co–Ni alloy and r GO.Stability tests,realized via longterm potential cycles and extended electrolysis,provided the confirmation of the exceptional durability of the catalyst,which originated from the confining effect of the N-doped carbon shell.This versatile method provides a strategy for designing stable non-precious metal electrocatalysts confined by carboncoating.
基金the China National Natural Science Foundation of China (Nos. 21722604, 21576122, 21376111)A Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)+1 种基金a scholarship from the China Scholarship Council (CSC)the Postgraduate Innovation Project of Jiangsu Province (NO. KYLX15_1067)
文摘High-quality graphene flakes have long been desirable for numerous applications including energy stor- age, printable electronics, and catalysis. In this contribution, we report a green, efficient, facile gas-driven exfoliation process for the preparation of high-quality graphene in large scale. The gas exfoliation process was realized by the interplay between the expansion of interlayer at high temperature and the gasifi- cation of liquid nitrogen within the interlayer. Detailed experiments demonstrated that the higher tem- perature was critical to the formation of fewer layers. The exfoliated graphene was proved to be of high quality. We further investigated the electrochemical behavior of this exfoliated graphene. As a result, this few-layered graphene demonstrated an enhanced capability as a supercapacitor, much higher than its counterpart parent material.
