CH_(4) storage associated with adsorbed natural gas(ANG)technology is an issue attracting great concern.Following the Advanced Research Project Agency-Energy(ARPA-E)targeted deliverable capacity of 315 cm^(3)·cm^...CH_(4) storage associated with adsorbed natural gas(ANG)technology is an issue attracting great concern.Following the Advanced Research Project Agency-Energy(ARPA-E)targeted deliverable capacity of 315 cm^(3)·cm^(-3)(STP),hundreds of thousands of materials have been experimentally or theoretically evaluated,while the best results still show a 35% gap from the target.Moreover,recent theoretical research reveals that the target is beyond the possibility that real materials can be designed.To get rid of the awkward situation,we make attempts on investigating the CH_(4) delivery performance under other operation conditions.Methods of raising the discharge temperature(to infinite high)or elevating the storage pressure(to 25 MPa)have been proved to show limited effectiveness.In this work,it is found that the ARPA-E target can be achieved by using a decreasing storage temperature strategy.By taking 280 CoRE(computation-ready,experimental)COFs(covalent organic frameworks)as ANG materials,when reduce the storage temperature to 190.6 K,the highest deliverable capacity can reach 392 cm^(3)·cm^(-3)(STP),and 16.1% CoRE COFs can surpass the target.The target is also achievable when storage at 220 K.Structure performance relationships study shows strong correlation between deliverable capacity and void fraction.Hence,120 hypothetical COFs are generated to ascertain the optimum void fraction.In addition,the performance of 2D-COFs can be greatly enhanced by increasing the interlayer spacings,e.g.CH_(4) deliverable capacity(storage at 190.6 K)of ATFG-COF can be improved from 239 to 411 cm^(3)·cm^(-3)(STP)when interlayer spacing is enlarged to 1.65 nm.展开更多
Herein, we describe a strategy for fabricating ordered mesoporous In2O3-reduced graphene oxide(r GO)nanocomposite through ultrasonic mixing, where ordered mesoporous In2O3 nanoparticles are synthesized via the nanocas...Herein, we describe a strategy for fabricating ordered mesoporous In2O3-reduced graphene oxide(r GO)nanocomposite through ultrasonic mixing, where ordered mesoporous In2O3 nanoparticles are synthesized via the nanocasting route by using mesoporous silica as a hard template, which possess ordered mesostructure with a large surface area of 81 m2g-1, and r GO nanosheets are synthesized from graphite via graphene oxide(GO) as intermediate. After coupled with r GO, mesoporous In2O3 could maintain its ordered mesostructure. We subsequently investigate the gas-sensing properties of all the In2O3 specimens with or without r GO for different gases. The results exhibit the ordered mesoporous In2O3-r GO nanocomposite possesses significantly enhanced response to ethanol even at low concentration levels, superior over pure mesoporous In2O3 nanoparticles. Similar strategy could be extended to other ordered mesoporous metal oxide–r GO nanocomposite for improving the gas-sensing property.展开更多
Highly sensitive and selective detection against specific target gases,especially at low-ppb(part per billion)level,remain a great number of challenges in gas sensor applications.In this paper,we first present an orde...Highly sensitive and selective detection against specific target gases,especially at low-ppb(part per billion)level,remain a great number of challenges in gas sensor applications.In this paper,we first present an ordered mesoporous NiFe_2O_4 for highly sensitive and selective detection against low-ppb toluene.A series of mesoporous NiFe_2O_4 materials were synthesized by templating from mesoporous silica KIT-6 and its framework thickness was reduced from 8.5 to 5 nm by varying the pore size of KIT-6 from 9.4 to 5.6 nm,accompanied with the increase of the specific surface area from 134 to 216 m^2g^(-1).The ordered mesoporous NiFe_2O_4 with both ultrathin framework of 5 nm and large specific surface area of up to 216 m^2g^(-1)exhibits a highest response(R_(gas)/R_(air)-1=77.3)toward 1,000 ppb toluene at 230℃ and is nearly 7.3 and 76.7 times higher than those for the NiFe_2O_4 replica with thick framework and its bulk counterpart respectively,which also possesses a quite low limit of detection(<2 ppb),and good selectivity.展开更多
The electrocatalytic activity for hydrogen evolution reaction(HER)is strongly correlated with active edge sites and resulting efficient charge transport capability.Here,we presented a facile two-step method to synthes...The electrocatalytic activity for hydrogen evolution reaction(HER)is strongly correlated with active edge sites and resulting efficient charge transport capability.Here,we presented a facile two-step method to synthesize 3 D hierarchical NiS2/MoS2 composite nanostructures on a carbon fiber paper(CFP)skeleton.The nanostructures distributed on CFP uniformly and composed of 2 D nanosheets,which would provide plenty of active edge sites and increase the HER activity.Electrochemical measurement suggests that the prepared NiS2/MoS2 exhibit great HER activity including a low overpotential of 102 m V,a small Tafel slope of 67 m V/dec,and a high double-layer capacity of 53.7 m F/cm2 in 1 M KOH aqueous solution.In addition,the HER activity is almost unchanged after galvanostatic technique with applied current densities of10 m A/cm2 for 20 h.展开更多
基金This work was supported by the Natural Science Foundation of China(21706106,51702137)the Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering(2020-KF-20)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX20_2236).
文摘CH_(4) storage associated with adsorbed natural gas(ANG)technology is an issue attracting great concern.Following the Advanced Research Project Agency-Energy(ARPA-E)targeted deliverable capacity of 315 cm^(3)·cm^(-3)(STP),hundreds of thousands of materials have been experimentally or theoretically evaluated,while the best results still show a 35% gap from the target.Moreover,recent theoretical research reveals that the target is beyond the possibility that real materials can be designed.To get rid of the awkward situation,we make attempts on investigating the CH_(4) delivery performance under other operation conditions.Methods of raising the discharge temperature(to infinite high)or elevating the storage pressure(to 25 MPa)have been proved to show limited effectiveness.In this work,it is found that the ARPA-E target can be achieved by using a decreasing storage temperature strategy.By taking 280 CoRE(computation-ready,experimental)COFs(covalent organic frameworks)as ANG materials,when reduce the storage temperature to 190.6 K,the highest deliverable capacity can reach 392 cm^(3)·cm^(-3)(STP),and 16.1% CoRE COFs can surpass the target.The target is also achievable when storage at 220 K.Structure performance relationships study shows strong correlation between deliverable capacity and void fraction.Hence,120 hypothetical COFs are generated to ascertain the optimum void fraction.In addition,the performance of 2D-COFs can be greatly enhanced by increasing the interlayer spacings,e.g.CH_(4) deliverable capacity(storage at 190.6 K)of ATFG-COF can be improved from 239 to 411 cm^(3)·cm^(-3)(STP)when interlayer spacing is enlarged to 1.65 nm.
基金supported by the National Natural Science Foundation of China(22178213)the Key Research and Development Program of Shaanxi Province(2022GY-196,2022GY-201,2022GY-184)+3 种基金the Innovation Capability Support Program of Shaanxi(2023KJXX-018)the Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(2022-K30)the Fundamental Research Funds for the Central Universities(GK202207007,GK202309002)the Open Project of Yunnan Precious Metals Laboratory Co.,Ltd(YPML-2023050246)。
基金supported by the National Natural Science Foundation of China(21006116,51362024)the Natural Science Foundation of Ningxia(NZ12111,NZ14010)the Prophase Research Special Project of the National Basic Research Program of China(2012CB723106)
文摘Herein, we describe a strategy for fabricating ordered mesoporous In2O3-reduced graphene oxide(r GO)nanocomposite through ultrasonic mixing, where ordered mesoporous In2O3 nanoparticles are synthesized via the nanocasting route by using mesoporous silica as a hard template, which possess ordered mesostructure with a large surface area of 81 m2g-1, and r GO nanosheets are synthesized from graphite via graphene oxide(GO) as intermediate. After coupled with r GO, mesoporous In2O3 could maintain its ordered mesostructure. We subsequently investigate the gas-sensing properties of all the In2O3 specimens with or without r GO for different gases. The results exhibit the ordered mesoporous In2O3-r GO nanocomposite possesses significantly enhanced response to ethanol even at low concentration levels, superior over pure mesoporous In2O3 nanoparticles. Similar strategy could be extended to other ordered mesoporous metal oxide–r GO nanocomposite for improving the gas-sensing property.
基金supported by the National First-Rate Discipline Construction Project of Ningxia(NXYLXK2017A04,2017CET02KY03,and 2017CET04KY05)the National Natural Science Foundation of China(51362024,21006116,and 51672138)+2 种基金the Foundation of State Key Laboratory of High-Efficiency Utilization of Coal and Green Chemical Engineering(2016–19)National Science Fund for Distinguished Young Scholars(21325105)the West Light Foundation of the Chinese Academy of Science
文摘Highly sensitive and selective detection against specific target gases,especially at low-ppb(part per billion)level,remain a great number of challenges in gas sensor applications.In this paper,we first present an ordered mesoporous NiFe_2O_4 for highly sensitive and selective detection against low-ppb toluene.A series of mesoporous NiFe_2O_4 materials were synthesized by templating from mesoporous silica KIT-6 and its framework thickness was reduced from 8.5 to 5 nm by varying the pore size of KIT-6 from 9.4 to 5.6 nm,accompanied with the increase of the specific surface area from 134 to 216 m^2g^(-1).The ordered mesoporous NiFe_2O_4 with both ultrathin framework of 5 nm and large specific surface area of up to 216 m^2g^(-1)exhibits a highest response(R_(gas)/R_(air)-1=77.3)toward 1,000 ppb toluene at 230℃ and is nearly 7.3 and 76.7 times higher than those for the NiFe_2O_4 replica with thick framework and its bulk counterpart respectively,which also possesses a quite low limit of detection(<2 ppb),and good selectivity.
基金financially supported by Key Research and Development Project of Hainan Province(No.ZDYF2018106)National Natural Science Foundation of China(Nos.51762012,51461014,and 51862006)Key Laboratory Open Project Fund of Hainan University(2018008).
文摘The electrocatalytic activity for hydrogen evolution reaction(HER)is strongly correlated with active edge sites and resulting efficient charge transport capability.Here,we presented a facile two-step method to synthesize 3 D hierarchical NiS2/MoS2 composite nanostructures on a carbon fiber paper(CFP)skeleton.The nanostructures distributed on CFP uniformly and composed of 2 D nanosheets,which would provide plenty of active edge sites and increase the HER activity.Electrochemical measurement suggests that the prepared NiS2/MoS2 exhibit great HER activity including a low overpotential of 102 m V,a small Tafel slope of 67 m V/dec,and a high double-layer capacity of 53.7 m F/cm2 in 1 M KOH aqueous solution.In addition,the HER activity is almost unchanged after galvanostatic technique with applied current densities of10 m A/cm2 for 20 h.
