Development of pore structures of activated carbon(AC)from activation of biomass with ZnCl_(2) relies on content and structure of cellulose/hemicellulose in the feedstock.Thermal pretreatment of biomass could induce d...Development of pore structures of activated carbon(AC)from activation of biomass with ZnCl_(2) relies on content and structure of cellulose/hemicellulose in the feedstock.Thermal pretreatment of biomass could induce dehydration and/or aromatization to change the structure of cellulose/hemicellulose.This might interfere with evolution of structures of AC,which was investigated herein via thermal pretreatment of willow branch(WB)from 200 to 360℃and the subsequent activation with ZnCl_(2) at 550℃.The results showed that thermal pretreatment at 360℃(WB-360)could lead to substantial pyrolysis to form biochar,with a yield of 31.9%,accompanying with nearly complete destruction of cellulose crystals and remarkably enhanced aromatic degree.However,cellulose residual in WB-360 could still be activated to form AC-360 with specific surface area of 1837.9 m~2·g^(-1),which was lower than that in AC from activation of untreated WB(AC-blank,2077.8 m~2·g^(-1)).Nonetheless,the AC-200 from activation of WB-200 had more developed pores(2113.9 m~2·g^(-1))and superior capability for adsorption of phenol,due to increased permeability of ZnCl_(2) to the largely intact cellulose structure in WB-200.The thermal pretreatment did increase diameters of micropores of AC but reduced the overall yield of AC(26.8%for AC-blank versus 18.0%for AC-360),resulting from accelerated cracking but reduced intensity of condensation.In-situ infrared characterization of the activation showed that ZnCl_(2) mainly catalyzed dehydration,dehydrogenation,condensation,and aromatization but not cracking,suppressing the formation of derivatives of cellulose and lignin in bio-oil.The thermal pretreatment formed phenolic-OH and C=O with higher chemical innerness,which changed the reaction network in activation,shifting morphology of fibrous structures in AC-blank to“melting surface”in AC-200 or AC-280.展开更多
Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electroche...Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.展开更多
The automatic collection of power grid situation information, along with real-time multimedia interaction between the front and back ends during the accident handling process, has generated a massive amount of power g...The automatic collection of power grid situation information, along with real-time multimedia interaction between the front and back ends during the accident handling process, has generated a massive amount of power grid data. While wireless communication offers a convenient channel for grid terminal access and data transmission, it is important to note that the bandwidth of wireless communication is limited. Additionally, the broadcast nature of wireless transmission raises concerns about the potential for unauthorized eavesdropping during data transmission. To address these challenges and achieve reliable, secure, and real-time transmission of power grid data, an intelligent security transmission strategy with sensor-transmission-computing linkage is proposed in this paper. The primary objective of this strategy is to maximize the confidentiality capacity of the system. To tackle this, an optimization problem is formulated, taking into consideration interruption probability and interception probability as constraints. To efficiently solve this optimization problem, a low-complexity algorithm rooted in deep reinforcement learning is designed, which aims to derive a suboptimal solution for the problem at hand. Ultimately, through simulation results, the validity of the proposed strategy in guaranteed communication security, stability, and timeliness is substantiated. The results confirm that the proposed intelligent security transmission strategy significantly contributes to the safeguarding of communication integrity, system stability, and timely data delivery.展开更多
The body channel based wireless power transfer(BC-WPT)method utilizes the human body as the medium to transfer power for bioelectronics,which can achieve a lower transmission loss due to its higher conductivity.Howeve...The body channel based wireless power transfer(BC-WPT)method utilizes the human body as the medium to transfer power for bioelectronics,which can achieve a lower transmission loss due to its higher conductivity.However,except for the channel length,different on-body loca-tions of the transmitter and receiver also influence the power supply performance.This paper fo-cuses on the wrist-to-forehead path to show the potential of BC-WPT for the brain bioelectronics such as the brain computer interface device.The channel characteristics from 10 MHz to 60 MHz are measured by a vector network analyzer(VNA)and a prototype BC-WPT system with differ-ent copper electrodes and the lowest power loss locates between-22 dB and-33 dB.Furthermore,the minimum path loss limit is simulated in Advanced Design System(ADS)software and the low-est optimum path loss can reach nearly-13 dB.Finally,a rectifier circuit is also built at the receiv-er side to harvest d.c.voltage.The results show that the open-circuit voltage(OCV)can reach 1.75 V with the transmitter of 50Ωoutput impedance supplying 5V_(pp)sine voltage at 60 MHz when adopt-ing 1 cm-diameter circular electrodes.展开更多
Highly selective binding of structurally similar substrates is common for biomolecular recognition,but is often challenging to realize in synthetic hosts.Herein,we report highly selective binding of methyl viologen ov...Highly selective binding of structurally similar substrates is common for biomolecular recognition,but is often challenging to realize in synthetic hosts.Herein,we report highly selective binding of methyl viologen over other analogues by an endo-functionalized naphthobox.X-ray single crystal structure and Density Functional Theory(DFT)calculations revealed that the endo-functionalized groups in the cavity of the naphthobox is important for the high binding selectivity through the formation of multiple C-H…N,C-H…π,andπ…πinteractions with methyl viologen.展开更多
Transition metal oxides(TMOs)have been thought of potential anodic materials for lithium-ion batteries(LIBs)owing to their intriguing properties.However,the limited conductivity and drastic volume change still hinder ...Transition metal oxides(TMOs)have been thought of potential anodic materials for lithium-ion batteries(LIBs)owing to their intriguing properties.However,the limited conductivity and drastic volume change still hinder their practical applications.Herein,a metal oxyacid salts-confined pyrolysis strategy is proposed to construct hierarchical porous metal oxide@carbon(MO@C,MO=MoO_(2),V_(2)O_(5),WO_(3))composites for solving the aforementioned problems.A water-evaporation-induced self-assembly mechanism has been put forward for fabricating the MO@polyvinyl pyrrolidone(PVP)@SiO_(2)precursors.After the following pyrolysis and etching process,small MO nanoparticles can be successfully encapsulated in the hierarchical porous carbon framework.Profiting from the synergistic effect of MO nanoparticles and highly conductive carbon framework,MO@C composites show excellent electrochemical properties.For example,the as-obtained MoO_(2)@C composite exhibits a large discharge capacity(1513.7 mAh·g^(−1)at 0.1 A·g^(−1)),good rate ability(443.5 mAh·g^(−1)at 5.0 A·g^(−1)),supernal long-lived stability(669.1 mAh·g^(−1)after 1000 cycles at 1.0 A·g^(−1)).This work will inspire the design of novel anode materials for high-performance LIBs.展开更多
基金supported by the National Natural Science Foundation of China(52276195)Program for Supporting Innovative Research from Jinan(202228072)Program of Agricultural Development from Shandong(SD2019NJ015)。
文摘Development of pore structures of activated carbon(AC)from activation of biomass with ZnCl_(2) relies on content and structure of cellulose/hemicellulose in the feedstock.Thermal pretreatment of biomass could induce dehydration and/or aromatization to change the structure of cellulose/hemicellulose.This might interfere with evolution of structures of AC,which was investigated herein via thermal pretreatment of willow branch(WB)from 200 to 360℃and the subsequent activation with ZnCl_(2) at 550℃.The results showed that thermal pretreatment at 360℃(WB-360)could lead to substantial pyrolysis to form biochar,with a yield of 31.9%,accompanying with nearly complete destruction of cellulose crystals and remarkably enhanced aromatic degree.However,cellulose residual in WB-360 could still be activated to form AC-360 with specific surface area of 1837.9 m~2·g^(-1),which was lower than that in AC from activation of untreated WB(AC-blank,2077.8 m~2·g^(-1)).Nonetheless,the AC-200 from activation of WB-200 had more developed pores(2113.9 m~2·g^(-1))and superior capability for adsorption of phenol,due to increased permeability of ZnCl_(2) to the largely intact cellulose structure in WB-200.The thermal pretreatment did increase diameters of micropores of AC but reduced the overall yield of AC(26.8%for AC-blank versus 18.0%for AC-360),resulting from accelerated cracking but reduced intensity of condensation.In-situ infrared characterization of the activation showed that ZnCl_(2) mainly catalyzed dehydration,dehydrogenation,condensation,and aromatization but not cracking,suppressing the formation of derivatives of cellulose and lignin in bio-oil.The thermal pretreatment formed phenolic-OH and C=O with higher chemical innerness,which changed the reaction network in activation,shifting morphology of fibrous structures in AC-blank to“melting surface”in AC-200 or AC-280.
基金financially supported by the Natural Science Foundation of Shandong Province (ZR2020QB132,ZR2020MB025)the Opening Project of State Key Laboratory of High Performance Ceramics and Superfine Microstructure (SKL202108SIC)the Taishan Scholar Program of Shandong Province (ts201712046)。
文摘Combination of CO_(2) capture using inorganic alkali with subsequently electrochemical conversion of the resultant HCO_(3)^(-)to high-value chemicals is a promising route of low cost and high efficiency.The electrochemical reduction of HCO_(3)^(-)is challenging due to the inaccessible of negatively charged molecular groups to the electrode surface.Herein,we adopt a comprehensive strategy to tackle this challenge,i.e.,cascade of in situ chemical conversion of HCO_(3)^(-)to CO_(2) and CO_(2) electrochemical reduction in a flow cell.With a tailored Ni-N-S single atom catalyst(SACs),where sulfur(S)atoms located in the second shell of Ni center,the CO_(2)electroreduction(CO_(2)ER)to CO is boosted.The experimental results and density functional theory(DFT)calculations reveal that the introduction of S increases the p electron density of N atoms near Ni atom,thereby stabilizing^(*)H over N and boosting the first proton coupled electron transfer process of CO_(2)ER,i.e.,^(*)+e^(-)+^(*)H+^(*)CO_(2)→^(*)COOH.As a result,the obtained catalyst exhibits a high faradaic efficiency(FE_(CO)~98%)and a low overpotential of 425 mV for CO production as well as a superior turnover frequency(TOF)of 47397 h^(-1),outcompeting most of the reported Ni SACs.More importantly,an extremely high FECOof 90%is achieved at 50 mA cm^(-2)in the designed membrane electrode assembly(MEA)cascade electrolyzer fed with liquid bicarbonate.This work not only highlights the significant role of the second coordination on the first coordination shell of the central metal for CO_(2)ER,but also provides an alternative and feasible strategy to realize the electrochemical conversion of HCO_(3)^(-)to high-value chemicals.
文摘The automatic collection of power grid situation information, along with real-time multimedia interaction between the front and back ends during the accident handling process, has generated a massive amount of power grid data. While wireless communication offers a convenient channel for grid terminal access and data transmission, it is important to note that the bandwidth of wireless communication is limited. Additionally, the broadcast nature of wireless transmission raises concerns about the potential for unauthorized eavesdropping during data transmission. To address these challenges and achieve reliable, secure, and real-time transmission of power grid data, an intelligent security transmission strategy with sensor-transmission-computing linkage is proposed in this paper. The primary objective of this strategy is to maximize the confidentiality capacity of the system. To tackle this, an optimization problem is formulated, taking into consideration interruption probability and interception probability as constraints. To efficiently solve this optimization problem, a low-complexity algorithm rooted in deep reinforcement learning is designed, which aims to derive a suboptimal solution for the problem at hand. Ultimately, through simulation results, the validity of the proposed strategy in guaranteed communication security, stability, and timeliness is substantiated. The results confirm that the proposed intelligent security transmission strategy significantly contributes to the safeguarding of communication integrity, system stability, and timely data delivery.
文摘The body channel based wireless power transfer(BC-WPT)method utilizes the human body as the medium to transfer power for bioelectronics,which can achieve a lower transmission loss due to its higher conductivity.However,except for the channel length,different on-body loca-tions of the transmitter and receiver also influence the power supply performance.This paper fo-cuses on the wrist-to-forehead path to show the potential of BC-WPT for the brain bioelectronics such as the brain computer interface device.The channel characteristics from 10 MHz to 60 MHz are measured by a vector network analyzer(VNA)and a prototype BC-WPT system with differ-ent copper electrodes and the lowest power loss locates between-22 dB and-33 dB.Furthermore,the minimum path loss limit is simulated in Advanced Design System(ADS)software and the low-est optimum path loss can reach nearly-13 dB.Finally,a rectifier circuit is also built at the receiv-er side to harvest d.c.voltage.The results show that the open-circuit voltage(OCV)can reach 1.75 V with the transmitter of 50Ωoutput impedance supplying 5V_(pp)sine voltage at 60 MHz when adopt-ing 1 cm-diameter circular electrodes.
基金financially supported by the National Natural Science Foundation of China(No.22125105)the Shenzhen Science and Technology Innovation Committee(No.JCYJ20180504165810828)+3 种基金Guangdong Provincial Key Laboratory of Catalysis(No.2020B121201002)Shenzhen“Pengcheng Scholar”Guangdong High-Level Personnel of Special Support Program(No.2019TX05C157)the Croucher Foundation。
文摘Highly selective binding of structurally similar substrates is common for biomolecular recognition,but is often challenging to realize in synthetic hosts.Herein,we report highly selective binding of methyl viologen over other analogues by an endo-functionalized naphthobox.X-ray single crystal structure and Density Functional Theory(DFT)calculations revealed that the endo-functionalized groups in the cavity of the naphthobox is important for the high binding selectivity through the formation of multiple C-H…N,C-H…π,andπ…πinteractions with methyl viologen.
基金the Taishan Scholar Project of Shandong Province(No.tsqn201909115)And this work was partly supported by Qingdao University of Science and Technology Hua Xue 201919(No.QUSTHX201919).
文摘Transition metal oxides(TMOs)have been thought of potential anodic materials for lithium-ion batteries(LIBs)owing to their intriguing properties.However,the limited conductivity and drastic volume change still hinder their practical applications.Herein,a metal oxyacid salts-confined pyrolysis strategy is proposed to construct hierarchical porous metal oxide@carbon(MO@C,MO=MoO_(2),V_(2)O_(5),WO_(3))composites for solving the aforementioned problems.A water-evaporation-induced self-assembly mechanism has been put forward for fabricating the MO@polyvinyl pyrrolidone(PVP)@SiO_(2)precursors.After the following pyrolysis and etching process,small MO nanoparticles can be successfully encapsulated in the hierarchical porous carbon framework.Profiting from the synergistic effect of MO nanoparticles and highly conductive carbon framework,MO@C composites show excellent electrochemical properties.For example,the as-obtained MoO_(2)@C composite exhibits a large discharge capacity(1513.7 mAh·g^(−1)at 0.1 A·g^(−1)),good rate ability(443.5 mAh·g^(−1)at 5.0 A·g^(−1)),supernal long-lived stability(669.1 mAh·g^(−1)after 1000 cycles at 1.0 A·g^(−1)).This work will inspire the design of novel anode materials for high-performance LIBs.