Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.H...Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.Here,we report one cobalt phosphide-based heterostructure anode(denoted as Co_(x)P-HS hereafter)to exhibit extremely robust alkaline OER at 500 mA cm^(−2).Together with home-made NiMoOx cathode,we could fabricate one efficient two-electrode overall water splitting system,based on which one photovoltaic-driven electrochemical(PV-EC)water splitting device was further constructed for robust solar-to-hydrogen(STH)conversion with efficiency of over∼27.10%under one sun illumination.The extraordinary OER stability of our catalyst was unraveled to predominantly result from all-for-one design of multiple structural parameters,where the quasi-in situ growth of catalyst is favorable to prevent physical exfoliation of catalyst,while the local structure featured with two-dimensional morphology,polymorphic heterostructure and sulfur-doping modulation is highly desirable for efficient charge transfer and surface catalysis,leading to excellent electrochemical stability.展开更多
Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic o...Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic oxygen evolution reaction(OER)is still shortage.Herein,we report remarkable promotion of OER performance on the NiFe‐based nanocomposite electrocatalyst via the synergy of multiple carbon‐based interface engineering.Specifically,carbon nanotubes were in situ grown on carbon fiber paper to improve the interface between CFP and NiFeO_(x)H_(y),and graphite carbon nanoparticles were in situ loaded and partly doped into the NiFeO_(x)H_(y) to modify the intergranular interface charge transfer and electronic structure of NiFeO_(x)H_(y).Consequently,the as‐obtained NiFeO_(x)H_(y)‐C/CNTs/CFP catalyst exhibited significantly enhanced electrocatalytic OER activity with an overpotential of 202 mV at 10 mA cm^(-2) in 1 mol L^(-1) KOH.Our work not only extends application of carbon materials but also provides an alternative strategy to develop highly efficient electrocatalysts.展开更多
The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal ...The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal nanoparticles aggregation during pyrolysis process. Herein, we reported the efficient synthesis of nitrogen doped carbon hollow nanospheres with cobalt nanoparticles （Co NP, ca. 10nm in size） distributed uniformly in the shell via pyrolysis of yolk-shell structured Zn-Co-ZIFs@polydopamine （PDA）. PDA acted as both protection layer and carbon source, which successfully prevented the aggregation of cobalt nanoparticles during high-temperature pyrolysis process. The Co NP and N containing carbon （Co NP/NC） hollow nanospheres were active for both oxygen evolution reaction （OER） and oxygen reduction reaction （ORR）, affording overpotential of 430 mV at 10 mA/cm2 for OER in 1 M KOH and comparable half-wave potential to that of Pt/C （0.80V vs RHE） for ORR in 0.1 M KOH. The superior performance of carbon hollow nanospheres for both OER and ORR was mainly attributed to its small metal nanoparticles, N-doping and hollow nanostructure. The protection and confinement effect that originated from PDA coating strategy could be extended to the synthesis of other hollow structured carbon materials, especially the ones with small metal nanoparticles.展开更多
Microorganisms have been essential in the natural world for millions of years,contributing significantly to environmental interaction.It has been disoverd that some bacteria are potential in geotechnical and environme...Microorganisms have been essential in the natural world for millions of years,contributing significantly to environmental interaction.It has been disoverd that some bacteria are potential in geotechnical and environmental engineering due to their outstanding ability of biomineralization.Therefore,how to train bacteria as special and professional“workers”for biomineralization is increasingly a key topic in related research fields.This article briefly introduces the methods that are commonly utilized to improve the environmental adaptability and mineralization efficiency of bacteria,including microbial domestication,microbial mutation breeding,microbial targeted screening,and bio-stimulation,which make great implications to advance the field of biomineralization.展开更多
Although conducting materials such as carbon nanotube and carbon fiber paper(CFP)have been extensively employed as support of electrocatalytic active sites,most of them are of poor catalytic functionality by themselve...Although conducting materials such as carbon nanotube and carbon fiber paper(CFP)have been extensively employed as support of electrocatalytic active sites,most of them are of poor catalytic functionality by themselves and undesirable stability during strong acid/alkaline environments or oxidation process.Here we report a novel one-dimensional(1D)nickel phosphide polymorphic heterostructure(denoted as NPPH)to work as one effective carbon-free functional support for loading of single-atom Ir water oxidation electrocatalyst.Specifically,the NPPH composed of both Ni12P5and Ni2P phases is not only active for robust alkaline water oxidation but also is of good stability and hydrophilicity for favorable loading of single-atom dispersed iridium.The NPPH supported single-atom Ir electrocatalyst(Ir/NPPH)is found to exhibit remarkably superior water oxidation activity with respect to the NPPH itself or CFP supported single-atom Ir catalyst(Ir/CFP),demonstrating the synergetic promotion effect between NPPH and single-atom Ir catalyst.Furthermore,the NPPH supported single-atom Ir catalyst can bear alkaline water oxidation for over 120 h at current density of 50 mA cm^(-2).The NPPH developed here is expected as functional support to composite with other water oxidation catalysts,as may be an alternative strategy of developing highly efficient carbon-free electrocatalysts.展开更多
Producing fuels or chemicals via electrochemical carbon dioxide reduction reaction(CO_(2)RR)with renewable electricity has attracted great research interest due to its potential of alleviating the environmental and en...Producing fuels or chemicals via electrochemical carbon dioxide reduction reaction(CO_(2)RR)with renewable electricity has attracted great research interest due to its potential of alleviating the environmental and energy issues in a carbon–neutral manner[1].The CO_(2)RR is a proton-coupled electron transfer process with the simultaneous participation of multiple protons and electrons[2].展开更多
Aberrant RNA splicing produces alternative isoforms of genes to facilitate tumor progression,yet how this process is regulated by oncogenic signal remains largely unknown.Here,we unveil that non-canonical activation o...Aberrant RNA splicing produces alternative isoforms of genes to facilitate tumor progression,yet how this process is regulated by oncogenic signal remains largely unknown.Here,we unveil that non-canonical activation of nuclear AURKA promotes an oncogenic RNA splicing of tumor suppressor RBM4 directed by m^(6)A reader YTHDC1 in lung cancer.Nuclear translocation of AURKA is a prerequisite for RNA aberrant splicing,specifically triggering RBM4 splicing from the full isoform(RBM4-FL)to the short isoform(RBM4-S)in a kinase-independent manner.展开更多
Application of differentiation therapy targeting cellular plasticity for the treatment of solid malignancies has been lagging.Nasopharyngeal carci noma(NPC)is a distinctive cancer with poor differe ntiatio n and high ...Application of differentiation therapy targeting cellular plasticity for the treatment of solid malignancies has been lagging.Nasopharyngeal carci noma(NPC)is a distinctive cancer with poor differe ntiatio n and high prevalenee of Epstein-Barr virus(EBV)infection.Here,we show that the expressi on of EBV latent protein LMP1 in duces dediffere ntiated and stem-like status with high plasticity through the transcriptional inhibition of CEBPA.Mechanistically,LMP1 upregulates STAT5A and recruits HDAC 1/2 to the CEBPA locus to reduce its histone acetylation.HDAC inhibition restored CEBPA expression,reversing cellular dedifferentiation and stem-like status in mouse xeno graft models.These fin dings provide a novel mecha nistic epigenetic-based in sight into virus-induced cellular plasticity and propose a promising concept of differentiation therapy in solid tumor by using HDAC inhibitors to target cellular plasticity.展开更多
We hypothesized that balancing the content of exogenous amino acids, especially lysine, to reduce protein content in swine diets could reduce nitrogen(N) pollution associated with animal husbandry. Two experiments(45 ...We hypothesized that balancing the content of exogenous amino acids, especially lysine, to reduce protein content in swine diets could reduce nitrogen(N) pollution associated with animal husbandry. Two experiments(45 d each experiment) were performed on weaned piglets(Duroc x Landrace x Yorkshire,28 d of age) to test this and to determine the optimal lysine to crude protein(Lys:CP) ratio in diet. In Exp. 1,12 piglets(6 replicates [n = 6]) were fed diets containing different levels of CP(17% and 20%) but the same level of Lys, Increased CP content resulted in significant increases(P < 0.05) of average daily gain(ADG), average daily feed intake(ADFI), and body weight(BW);but did not affect the feed to gain ratio. In Exp. 2,24 piglets(8 replicates [n = 8]) were fed 1 of 3 diets as follows: 1) 20% CP with a regular Lys:CP ratio(6.23%, control);2) 17% CP with a reduced Lys:CP ratio(6.14%, LL);or 3) 17% CP with a standard Lys:CP ratio(7.32%, SL). The ADG, final BW, serum concentrations of growth hormone and insulin-like growth factor-1, villus height in the jejunum, and villus height to crypt depth ratio were the lowest in piglets fed LL diet, whereas blood urea N concentration was the lowest and the value of lipase activity was the highest in the piglets fed SL diet. The SL diet did not affect growth performance,intestinal morphology, or serum hormone concentrations, indicating that reduced dietary N with a high Lys:CP ratio can efficiently reduce dietary N excretion without negatively affecting weaned piglets.展开更多
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (XDB0600100)the National Key R&D Program of China (2020YFA0406100)+1 种基金the National Natural Science Foundation of China (21925206)National Natural Science Foundation of China (22332005)
文摘Development of non-noble-metal electrocatalysts with robust oxygen evolution reaction(OER)at the industrially required current density is desirable but still lacking for promising industrial-scale water electrolysis.Here,we report one cobalt phosphide-based heterostructure anode(denoted as Co_(x)P-HS hereafter)to exhibit extremely robust alkaline OER at 500 mA cm^(−2).Together with home-made NiMoOx cathode,we could fabricate one efficient two-electrode overall water splitting system,based on which one photovoltaic-driven electrochemical(PV-EC)water splitting device was further constructed for robust solar-to-hydrogen(STH)conversion with efficiency of over∼27.10%under one sun illumination.The extraordinary OER stability of our catalyst was unraveled to predominantly result from all-for-one design of multiple structural parameters,where the quasi-in situ growth of catalyst is favorable to prevent physical exfoliation of catalyst,while the local structure featured with two-dimensional morphology,polymorphic heterostructure and sulfur-doping modulation is highly desirable for efficient charge transfer and surface catalysis,leading to excellent electrochemical stability.
文摘Interface engineering has been widely investigated to regulate the structure and performance of electrodes and photoelectrodes,but the investigation of multiple carbon interface modifications on the electrocatalytic oxygen evolution reaction(OER)is still shortage.Herein,we report remarkable promotion of OER performance on the NiFe‐based nanocomposite electrocatalyst via the synergy of multiple carbon‐based interface engineering.Specifically,carbon nanotubes were in situ grown on carbon fiber paper to improve the interface between CFP and NiFeO_(x)H_(y),and graphite carbon nanoparticles were in situ loaded and partly doped into the NiFeO_(x)H_(y) to modify the intergranular interface charge transfer and electronic structure of NiFeO_(x)H_(y).Consequently,the as‐obtained NiFeO_(x)H_(y)‐C/CNTs/CFP catalyst exhibited significantly enhanced electrocatalytic OER activity with an overpotential of 202 mV at 10 mA cm^(-2) in 1 mol L^(-1) KOH.Our work not only extends application of carbon materials but also provides an alternative strategy to develop highly efficient electrocatalysts.
文摘The pyrolysis under inert atmosphere has been widely used for the synthesis of metal containing heteroatoms doped carbon materials, versatile catalysts for various reactions. However, it is difficult to prevent metal nanoparticles aggregation during pyrolysis process. Herein, we reported the efficient synthesis of nitrogen doped carbon hollow nanospheres with cobalt nanoparticles （Co NP, ca. 10nm in size） distributed uniformly in the shell via pyrolysis of yolk-shell structured Zn-Co-ZIFs@polydopamine （PDA）. PDA acted as both protection layer and carbon source, which successfully prevented the aggregation of cobalt nanoparticles during high-temperature pyrolysis process. The Co NP and N containing carbon （Co NP/NC） hollow nanospheres were active for both oxygen evolution reaction （OER） and oxygen reduction reaction （ORR）, affording overpotential of 430 mV at 10 mA/cm2 for OER in 1 M KOH and comparable half-wave potential to that of Pt/C （0.80V vs RHE） for ORR in 0.1 M KOH. The superior performance of carbon hollow nanospheres for both OER and ORR was mainly attributed to its small metal nanoparticles, N-doping and hollow nanostructure. The protection and confinement effect that originated from PDA coating strategy could be extended to the synthesis of other hollow structured carbon materials, especially the ones with small metal nanoparticles.
基金support from the National Natural Science Foundation of China(Grant No.52078085)Chongqing Planning and Natural Resources Bureau(No.KJ-2021048).
文摘Microorganisms have been essential in the natural world for millions of years,contributing significantly to environmental interaction.It has been disoverd that some bacteria are potential in geotechnical and environmental engineering due to their outstanding ability of biomineralization.Therefore,how to train bacteria as special and professional“workers”for biomineralization is increasingly a key topic in related research fields.This article briefly introduces the methods that are commonly utilized to improve the environmental adaptability and mineralization efficiency of bacteria,including microbial domestication,microbial mutation breeding,microbial targeted screening,and bio-stimulation,which make great implications to advance the field of biomineralization.
基金supported by the National Natural Science Foundation of China(21925206)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA 21000000)+1 种基金the National Key R&D Program of China(2020YFA0406100)the Liaoning provincial Natural Science Foundation of China(2020-BS-014)。
文摘Although conducting materials such as carbon nanotube and carbon fiber paper(CFP)have been extensively employed as support of electrocatalytic active sites,most of them are of poor catalytic functionality by themselves and undesirable stability during strong acid/alkaline environments or oxidation process.Here we report a novel one-dimensional(1D)nickel phosphide polymorphic heterostructure(denoted as NPPH)to work as one effective carbon-free functional support for loading of single-atom Ir water oxidation electrocatalyst.Specifically,the NPPH composed of both Ni12P5and Ni2P phases is not only active for robust alkaline water oxidation but also is of good stability and hydrophilicity for favorable loading of single-atom dispersed iridium.The NPPH supported single-atom Ir electrocatalyst(Ir/NPPH)is found to exhibit remarkably superior water oxidation activity with respect to the NPPH itself or CFP supported single-atom Ir catalyst(Ir/CFP),demonstrating the synergetic promotion effect between NPPH and single-atom Ir catalyst.Furthermore,the NPPH supported single-atom Ir catalyst can bear alkaline water oxidation for over 120 h at current density of 50 mA cm^(-2).The NPPH developed here is expected as functional support to composite with other water oxidation catalysts,as may be an alternative strategy of developing highly efficient carbon-free electrocatalysts.
基金supported by the National Natural Science Foundation of China(22179015,21872142,and 21802141)the Fundamental Research Funds for the Central Universities(3132022216 and 3132022217)+2 种基金the China Postdoctoral Science Foundation(2021M700651)the open fund of the state key laboratory of molecular reaction dynamics in DICP,CAS(SKLMRD-K202414)the Large Instruments and Facilities Shared Foundation of Dalian Maritime University。
文摘Producing fuels or chemicals via electrochemical carbon dioxide reduction reaction(CO_(2)RR)with renewable electricity has attracted great research interest due to its potential of alleviating the environmental and energy issues in a carbon–neutral manner[1].The CO_(2)RR is a proton-coupled electron transfer process with the simultaneous participation of multiple protons and electrons[2].
基金We thank Quentin Liu’s lab members for their critical comments and technical support.We thank Eric W.-F.Lam for his critical reading of the manuscript and insightful suggestions.This research work was supported by the National Natural Science Foundation of China(No.81820108024 to Q.L.,No.81630005 to Q.L.,No.81830088 to Y.W.,No.81873441 to B.-L.J.,No.82103659 to S.-S.L.,No.8210113819 to Y.-F.Q.,No.81972786 to J.X.,No.82003141 to F.P.,No.82002960 to B.C.,No.31801100 to X.-.D.D.)National Key R&D Program of China(2019YFA0110300 to Q.L.and 2017YFA0505600-04 to Q.L.)+12 种基金Program for Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(No.IRT_17R15)Innovative Research Team in University of Liaoning(No.LT2017001 to Q.L.)Heilongjiang Postdoctoral Fund(No.LBH-Z20074 to S.-S.L.)Harbin Medical University Doctor Green Seedling Ground-breaking Project(No.QMPT-1909 to S.-S.L.)the Natural Science Foundation of Liaoning(No.2019-BS-081 to F.P.)the“Seedling cultivation”program for young scientific and technological talents of Liaoning(No.LZ2020044 to F.P.,No.LZ2019067 to B.C.)Dalian Science and Technology program-The central government guiding local funding projects for scientific and technological development(2021 to F.P.)Dalian High-level Talents Innovation Support Program-Young Science and Technology Star(2021RQ004 to B.C.)the program for climbing Scholars of Liaoning,the Science and Technology Innovation Foundation of Dalian(No.2020JJ25CY008 to Q.L.)International Scientific and Technological Cooperation of Dalian(2015F11GH095 to Q.L.)the Natural Science Foundation of Guangdong(2016A030311038 and 2017A030313608 to Q.L.)the Science and Technology Planning Project of Guangzhou(No.201804020044 to Q.L.)the Scientific Research Project of Guangzhou(No.201904010492 to B.-L.J.).
文摘Aberrant RNA splicing produces alternative isoforms of genes to facilitate tumor progression,yet how this process is regulated by oncogenic signal remains largely unknown.Here,we unveil that non-canonical activation of nuclear AURKA promotes an oncogenic RNA splicing of tumor suppressor RBM4 directed by m^(6)A reader YTHDC1 in lung cancer.Nuclear translocation of AURKA is a prerequisite for RNA aberrant splicing,specifically triggering RBM4 splicing from the full isoform(RBM4-FL)to the short isoform(RBM4-S)in a kinase-independent manner.
基金supported by National Key R&D Program of China(2019YFA0110300,2017YFA0505600-04 to Q.L.)Innovative Research Team in University of Ministry of Education of China(IRT_17R15 to Q.L.)+7 种基金National Natural Science Foundation of China(81630005,81573025 to Q.L.,81773166 to Z.W.,81702683 to J.X.,81972594 to M.Y.,81402445 to C.W.,81502579 to Z.H.)Natural Science Foundation of Guangdong(2017A030313608 to Q.L,2018A0303130299,2020A1515010608 to M.Y.)the Science and Technology Planning Project of Guangzhou(201804020044 to Q.L.)the Key Project of Liaoning Natural Science Funding of China(201702031 to Q.L.)Fundamental Research Funds for the Central Universities(I9ykpy187 to M.Y.).EW-FL's work is supported by MRC(MR/N012097/1)CRUK(Al 2011)Breast Cancer Now(2012MayPR070,2012NovPhD016)the Cancer Research UK Imperial Centre,Imperial ECMC,and NIHR Imperial BRC.
文摘Application of differentiation therapy targeting cellular plasticity for the treatment of solid malignancies has been lagging.Nasopharyngeal carci noma(NPC)is a distinctive cancer with poor differe ntiatio n and high prevalenee of Epstein-Barr virus(EBV)infection.Here,we show that the expressi on of EBV latent protein LMP1 in duces dediffere ntiated and stem-like status with high plasticity through the transcriptional inhibition of CEBPA.Mechanistically,LMP1 upregulates STAT5A and recruits HDAC 1/2 to the CEBPA locus to reduce its histone acetylation.HDAC inhibition restored CEBPA expression,reversing cellular dedifferentiation and stem-like status in mouse xeno graft models.These fin dings provide a novel mecha nistic epigenetic-based in sight into virus-induced cellular plasticity and propose a promising concept of differentiation therapy in solid tumor by using HDAC inhibitors to target cellular plasticity.
基金supported by the China Basic Research Program (#2013CB127301)National Natural Science Foundation of China (31472106, 31501964)+5 种基金Natural Science Foundation of Hunan Province of China (2018JJ3579)Ministry of Science and Technology of the People’s Republic of China (2013BAD21B04)Key Programs of frontier scientific research of the Chinese Academy of Sciences (QYZDY-SSW-SMC008)Youth Innovation Team Project of ISA,CAS (2017QNCXTD_TBE)China Agriculture Research System (CARS-35)the Public Service Technology Center,Institute of Subtropical Agriculture, Chinese Academy of Sciences
文摘We hypothesized that balancing the content of exogenous amino acids, especially lysine, to reduce protein content in swine diets could reduce nitrogen(N) pollution associated with animal husbandry. Two experiments(45 d each experiment) were performed on weaned piglets(Duroc x Landrace x Yorkshire,28 d of age) to test this and to determine the optimal lysine to crude protein(Lys:CP) ratio in diet. In Exp. 1,12 piglets(6 replicates [n = 6]) were fed diets containing different levels of CP(17% and 20%) but the same level of Lys, Increased CP content resulted in significant increases(P < 0.05) of average daily gain(ADG), average daily feed intake(ADFI), and body weight(BW);but did not affect the feed to gain ratio. In Exp. 2,24 piglets(8 replicates [n = 8]) were fed 1 of 3 diets as follows: 1) 20% CP with a regular Lys:CP ratio(6.23%, control);2) 17% CP with a reduced Lys:CP ratio(6.14%, LL);or 3) 17% CP with a standard Lys:CP ratio(7.32%, SL). The ADG, final BW, serum concentrations of growth hormone and insulin-like growth factor-1, villus height in the jejunum, and villus height to crypt depth ratio were the lowest in piglets fed LL diet, whereas blood urea N concentration was the lowest and the value of lipase activity was the highest in the piglets fed SL diet. The SL diet did not affect growth performance,intestinal morphology, or serum hormone concentrations, indicating that reduced dietary N with a high Lys:CP ratio can efficiently reduce dietary N excretion without negatively affecting weaned piglets.
