Background:Alpha/beta hydrolase domain-containing protein 17C(ABHD17C)is a depalmitoylation enzyme that removes the S-palmitoylation of targeted proteins.The hepatocellular carcinoma(HCC)cells SNU449 and Hep3B use ABH...Background:Alpha/beta hydrolase domain-containing protein 17C(ABHD17C)is a depalmitoylation enzyme that removes the S-palmitoylation of targeted proteins.The hepatocellular carcinoma(HCC)cells SNU449 and Hep3B use ABHD17C as an oncogene;however,the exact mechanism of this action is yet unknown.Methods:The expression of ABHD17C in liver cancer tissues was analyzed by bioinformatics,and the expression of ABHD17C in clinical liver cancer tissues and adjacent normal tissues was detected.Then,the proliferative viability of HCC cells after overexpression or knockdown of ABHD17C was examined,and pyroptosis and apoptosis proteins were detected.Results:ABHD17C was overexpressed in human HCC tissues as well as numerous HCC cell lines.Depletion of ABHD17C caused reduced viability,cell cycle arrest,and defective invasion and migration in HCC cells,while overexpression of ABHD17C exhibited the opposite effect.Moreover,we discovered that the knockdown of ABHD17C resulted in enhanced apoptotic and pyroptotic phenotypes of HCC cells,whereas overexpression of ABHD17C attenuated such phenotypes.Conclusions:It suggests that ABHD17C contributes to HCC carcinogenesis,making it a promising target for medication treatment.展开更多
Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM,...Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM, XPS and TG techniques. We set the products selectivity as a function of butane conversion over various phosphate loading, and it is found that the PoCNT catalyst with the 0.8% phosphate weight loading(0.8PoCNT) exhibits the best catalytic performance. When the phosphate loading is higher than 0.8 wt%, the difference of catalytic activity among the PoCNT catalysts is neglectable. Consequently, the ODH of n-butane over the 0.8PoCNT catalyst is particularly discussed via changing the reaction conditions including reaction temperatures, residence time and n-butane/O;ratios. The interacting mechanism of phosphate with the oxygen functional groups on the CNT surface is also proposed.展开更多
The ethanol oxidation reaction(EOR)is crucial in direct alcohol fuel cells and chemical production.However,the electro-oxidation of ethanol molecules to produce acetaldehyde and carbon monoxide can poison the active s...The ethanol oxidation reaction(EOR)is crucial in direct alcohol fuel cells and chemical production.However,the electro-oxidation of ethanol molecules to produce acetaldehyde and carbon monoxide can poison the active sites of nanocatalysts,resulting in reduced performance and posing challenges in achieving high activity and selectivity for ethanol oxidation.In this study,we employed a dynamic seed-mediated method to precisely modify highly dispersed Ru sites onto well-defined Pd nanocrystals.The oxyphilic Ru sites serve as"OH valves",regulating water dissociation,while the surrounding Pd atomic arrangements control electronic states for the oxidation dehydrogenation of carbonaceous intermediates.Specifically,Ru0.040@Pd nanocubes(Ru:Pd=0.04 at.%),featuring(100)facets in Ru-Pd4 configurations,demonstrate an outstanding mass activity of 6.53 A·mgPd^(-1) in EOR under alkaline conditions,which is 6.05 times higher than that of the commercial Pd/C catalyst(1.08 A·mgPd-1).Through in-situ experiments and theoretical investigations,we elucidate that the hydrophilic Ru atoms significantly promote the dynamic evolution of H_(2)O dissociation into OHads species,while the electron redistribution from Ru to adjacent Pd concurrently adjusts the selective oxidation of C_(2) intermediates.This host-guest interaction accelerates the subsequent oxidation of carbonaceous intermediates(CH_(3)CO_(ads))to acetate,while preventing the formation of toxic*CHx and*CO species,which constitutes the rate-determining step.展开更多
Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developin...Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains challenging.Herein,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the surface.These NWs possess uniform sizes and well-controlled atomic arrangements.Compared to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based catalysts.Additionally,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/C.The ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.展开更多
Tremendous progress has been made on aromatic fusion of acenaphthylene towards organic semiconductors.However,scarce studies focus on the functionalization of acenaphthylene without resort to aromatic extension,althou...Tremendous progress has been made on aromatic fusion of acenaphthylene towards organic semiconductors.However,scarce studies focus on the functionalization of acenaphthylene without resort to aromatic extension,although vinylene double bond is highly reactive ascribed to the ring strain of the fused cyclopentene.Herein,for the first time we employ copper-promoted domino cyanation/Ullmann coupling to achieve a series of difunctionalized acenaphthylene imides(ANIs)with varied optoelectronic properties.Both Ullmann homocoupling and crosscoupling can be combined with cyanation for difunctionalization of ANIs.The introduction of cyano groups influences oppositely not only the energy levels but also the antiaromaticity of the fivemembered rings in ANIs relative to the dimethylamino substituent due to the electron donating or withdrawing effects.By altering the functional units,the optical and electrical characteristics have been tailored rationally;thus p,n or ambipolar semiconducting properties can be achieved for the ANI derivatives.This article opens up possibilities to the development of organic semiconducting materials based on ANIs without aromatic extension,which is promising for applications in organic electronics.展开更多
Fine regulation of geometric structures has great promise to acquire specific electronic structures and improve the catalytic performance of single-atom catalysts,yet it remains a challenge.Herein,a novel seed encapsu...Fine regulation of geometric structures has great promise to acquire specific electronic structures and improve the catalytic performance of single-atom catalysts,yet it remains a challenge.Herein,a novel seed encapsulation–decomposition strategy is proposed for the geometric distortion engineering and thermal atomization of a series of Cu-N_(x)/S moieties anchored on carbon supports.During pyrolysis,seeds(Cu^(2+),CuO,or Cu_(7)S_(4) nanoparticles)confined in metal organic framework can accommodate single Cu atoms with Cu–N or Cu–S coordination bonds and simultaneously induce C–S or C–N bond cleavage in the second coordination shell of Cu centers,which are identified to manipulate the distortion degree of Cu-N_(x)/S moieties.The severely distorted Cu-N3S molecular structure endows the resultant catalyst with excellent oxygen reduction reaction activity(E_(1/2)=0.885 V)and zinc-air battery performance(peak power density of 210 mW·cm^(−2)),outperforming the asymmetrical and symmetrical Cu-N4 structures.A combined experimental and theoretical study reveals that the geometric distortion of Cu-N_(x)/S moieties creates uneven charge distribution by a unique topological correlation effect,which increases the metal charge and shifts the d-band center toward the Fermi level,thereby optimizing the inter-mediate adsorption energy.展开更多
基金supported by the Quanzhou High-Level Talents Project(2021C048R).
文摘Background:Alpha/beta hydrolase domain-containing protein 17C(ABHD17C)is a depalmitoylation enzyme that removes the S-palmitoylation of targeted proteins.The hepatocellular carcinoma(HCC)cells SNU449 and Hep3B use ABHD17C as an oncogene;however,the exact mechanism of this action is yet unknown.Methods:The expression of ABHD17C in liver cancer tissues was analyzed by bioinformatics,and the expression of ABHD17C in clinical liver cancer tissues and adjacent normal tissues was detected.Then,the proliferative viability of HCC cells after overexpression or knockdown of ABHD17C was examined,and pyroptosis and apoptosis proteins were detected.Results:ABHD17C was overexpressed in human HCC tissues as well as numerous HCC cell lines.Depletion of ABHD17C caused reduced viability,cell cycle arrest,and defective invasion and migration in HCC cells,while overexpression of ABHD17C exhibited the opposite effect.Moreover,we discovered that the knockdown of ABHD17C resulted in enhanced apoptotic and pyroptotic phenotypes of HCC cells,whereas overexpression of ABHD17C attenuated such phenotypes.Conclusions:It suggests that ABHD17C contributes to HCC carcinogenesis,making it a promising target for medication treatment.
基金supported by the National Natural Science Foundation of China(No.91545110,21573254,21203214,21133010,21473223,21261160487,51221264)the Institute of Metal Research,Youth Innovation Promotion Association(CAS)the Sinopec China and the Strategic Priority Research Program of the Chinese Academy of Sciences,Grant No.XDA09030103
文摘Catalytic performance of phosphate-modified carbon nanotube(PoCNT) catalysts for oxidative dehydrogenation(ODH) of n-butane has been systematically investigated. The Po CNT catalysts are characterized by SEM, TEM, XPS and TG techniques. We set the products selectivity as a function of butane conversion over various phosphate loading, and it is found that the PoCNT catalyst with the 0.8% phosphate weight loading(0.8PoCNT) exhibits the best catalytic performance. When the phosphate loading is higher than 0.8 wt%, the difference of catalytic activity among the PoCNT catalysts is neglectable. Consequently, the ODH of n-butane over the 0.8PoCNT catalyst is particularly discussed via changing the reaction conditions including reaction temperatures, residence time and n-butane/O;ratios. The interacting mechanism of phosphate with the oxygen functional groups on the CNT surface is also proposed.
基金supported by the National Natural Science Foundation of China(No.22275009)SINOPEC(Contact No.421028)Fundamental Research Funds for the Central Universities(No.XK2020-02).
文摘The ethanol oxidation reaction(EOR)is crucial in direct alcohol fuel cells and chemical production.However,the electro-oxidation of ethanol molecules to produce acetaldehyde and carbon monoxide can poison the active sites of nanocatalysts,resulting in reduced performance and posing challenges in achieving high activity and selectivity for ethanol oxidation.In this study,we employed a dynamic seed-mediated method to precisely modify highly dispersed Ru sites onto well-defined Pd nanocrystals.The oxyphilic Ru sites serve as"OH valves",regulating water dissociation,while the surrounding Pd atomic arrangements control electronic states for the oxidation dehydrogenation of carbonaceous intermediates.Specifically,Ru0.040@Pd nanocubes(Ru:Pd=0.04 at.%),featuring(100)facets in Ru-Pd4 configurations,demonstrate an outstanding mass activity of 6.53 A·mgPd^(-1) in EOR under alkaline conditions,which is 6.05 times higher than that of the commercial Pd/C catalyst(1.08 A·mgPd-1).Through in-situ experiments and theoretical investigations,we elucidate that the hydrophilic Ru atoms significantly promote the dynamic evolution of H_(2)O dissociation into OHads species,while the electron redistribution from Ru to adjacent Pd concurrently adjusts the selective oxidation of C_(2) intermediates.This host-guest interaction accelerates the subsequent oxidation of carbonaceous intermediates(CH_(3)CO_(ads))to acetate,while preventing the formation of toxic*CHx and*CO species,which constitutes the rate-determining step.
基金the National Natural Science Foundation of China(No.22275009)SINOPEC(contact No.421028)Fundamental Research Funds for the Central Universities(No.XK2020-02).
文摘Increasing the utilization efficiency of platinum is critical for advancing proton exchange-membrane fuel cells(PEMFCs).Despite extensive research on catalysts for the cathodic oxygen reduction reaction(ORR),developing highly active and durable Pt-based catalysts that can suppress surface dealloying in corrosive acid conditions remains challenging.Herein,we report a facile synthesis of bimetallic ultrathin PtM(M=Mo,W,and Cr)nanowires(NWs)composed of group VI B transition metal atomic sites anchored on the surface.These NWs possess uniform sizes and well-controlled atomic arrangements.Compared to PtW and PtCr catalysts,the PtMo0.05 NWs exhibit the highest half-wave potential of 0.935 V and a mass activity of 1.43 A·mgPt^(−1).Remarkably,they demonstrate a remarkable 23.8-fold enhancement in mass activity compared to commercial Pt/C for ORR,surpassing previously reported Pt-based catalysts.Additionally,the PtMo NWs cathode in membrane electrode assembly tests achieves a remarkable peak power density of 1.443 W·cm^(−2)(H_(2)-O_(2)conditions at 80℃),which is 1.09 times that of commercial Pt/C.The ligand effect in the bimetallic surface not only facilitates strong coupling between Mo(4d)and Pt(5d)atomic orbitals to hinder atom leaching but also modulates the d-states of active site,significantly optimizing the adsorption of key oxygen(*O and*OH)species and accelerating the rate-determining step in ORR pathways.
基金supported by the Fundamental Research Funds for the Central Universities(buctrc202103 and buctrc202128)the National Natural Science Foundation of China(52103200,22171019,21975263 and 52273167)+4 种基金SINOPEC(222131)the Open Funds of the State Key Laboratory of Optoelectronic Materials and Technologies(Sun Yat-sen University)the State Key Laboratory of Fine Chemicals(KF2201,Dalian University of Technology)the State Key Laboratory of Luminescent Materials and Devices(2022-skllmd-14)the State Key Laboratory of Supramolecular Structure and Materials(SKLSSM2022036)。
基金supported by the Fundamental Research Funds for the Central Universities(buctrc202103,buctrc202128)the National Natural Science Foundation of China(21975263,22171019,52103200)+4 种基金SINOPEC(222131)the Open Project Program of Wuhan National Laboratory for Optoelectronics(2021WNLOKF005)the State Key Laboratory of Fine Chemicals(KF2201,Dalian University of Technology)the State Key Laboratory of Luminescent Materials and Devices(2022skllmd-14)the State Key Laboratory of Supramolecular Structure and Materials(SKLSSM2022036)。
文摘Tremendous progress has been made on aromatic fusion of acenaphthylene towards organic semiconductors.However,scarce studies focus on the functionalization of acenaphthylene without resort to aromatic extension,although vinylene double bond is highly reactive ascribed to the ring strain of the fused cyclopentene.Herein,for the first time we employ copper-promoted domino cyanation/Ullmann coupling to achieve a series of difunctionalized acenaphthylene imides(ANIs)with varied optoelectronic properties.Both Ullmann homocoupling and crosscoupling can be combined with cyanation for difunctionalization of ANIs.The introduction of cyano groups influences oppositely not only the energy levels but also the antiaromaticity of the fivemembered rings in ANIs relative to the dimethylamino substituent due to the electron donating or withdrawing effects.By altering the functional units,the optical and electrical characteristics have been tailored rationally;thus p,n or ambipolar semiconducting properties can be achieved for the ANI derivatives.This article opens up possibilities to the development of organic semiconducting materials based on ANIs without aromatic extension,which is promising for applications in organic electronics.
基金supported by the National Natural Science Foundation of China(Nos.21701005 and 21903001)the Fundamental Research Funds for the Central Universities(No.XK2020-02)China Petroleum&Chemical Corporation(SINOPEC)(No.421028)。
文摘Fine regulation of geometric structures has great promise to acquire specific electronic structures and improve the catalytic performance of single-atom catalysts,yet it remains a challenge.Herein,a novel seed encapsulation–decomposition strategy is proposed for the geometric distortion engineering and thermal atomization of a series of Cu-N_(x)/S moieties anchored on carbon supports.During pyrolysis,seeds(Cu^(2+),CuO,or Cu_(7)S_(4) nanoparticles)confined in metal organic framework can accommodate single Cu atoms with Cu–N or Cu–S coordination bonds and simultaneously induce C–S or C–N bond cleavage in the second coordination shell of Cu centers,which are identified to manipulate the distortion degree of Cu-N_(x)/S moieties.The severely distorted Cu-N3S molecular structure endows the resultant catalyst with excellent oxygen reduction reaction activity(E_(1/2)=0.885 V)and zinc-air battery performance(peak power density of 210 mW·cm^(−2)),outperforming the asymmetrical and symmetrical Cu-N4 structures.A combined experimental and theoretical study reveals that the geometric distortion of Cu-N_(x)/S moieties creates uneven charge distribution by a unique topological correlation effect,which increases the metal charge and shifts the d-band center toward the Fermi level,thereby optimizing the inter-mediate adsorption energy.