Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In p...Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In particular,an unstable cathode–electrolyte interphase(CEI)leads to successive electrolyte side reactions,transition metal leaching and rapid capacity decay,which tends to be exacerbated under high-voltage conditions.Therefore,constructing dense and stable CEIs are crucial for high-performance SIBs.This work reports localized high-concentration electrolyte by incorporating a highly oxidation-resistant sulfolane solvent with non-solvent diluent 1H,1H,5H-octafluoropentyl-1,1,2,2-tetrafluoroethyl ether,which exhibited excellent oxidative stability and was able to form thin,dense and homogeneous CEI.The excellent CEI enabled the O3-type layered oxide cathode NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)(NaNMF)to achieve stable cycling,with a capacity retention of 79.48%after 300 cycles at 1 C and 81.15%after 400 cycles at 2 C with a high charging voltage of 4.2 V.In addition,its nonflammable nature enhances the safety of SIBs.This work provides a viable pathway for the application of sulfolane-based electrolytes on SIBs and the design of next-generation high-voltage electrolytes.展开更多
The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic ...The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to nanoparticles.Therefore,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C catalysts.Accordingly,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation strategy.We found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe center.The as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,respectively.Moreover,the catalyst also represents excellent durability exceeding that of Fe–N–C SA catalyst.The practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery device.Our work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.展开更多
This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate,lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate.The polymerization of MMA was initiat...This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate,lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate.The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism.LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte.Normally,lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer,a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization.However,the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant.The as-prepared poly-methyl methacrylate-based polymer electrolyte has a high ionic conductivity(1.19×10^(−3)S cm^(−1)),a wide electrochemical stability window(5 V vs Li^(+)/Li),and a high Li ion transference number(t_(Li^(+)))of 0.74 at room temperature(RT).Moreover,this polymerization-derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode,which enabled the Li symmetric cell to achieve a long-term cycling performance at 0.2 mAh cm^(−2)for 2800 h.The LiFePO_(4)battery with polymerization-derived polymer electrolyte-modified Li metal anode shows a capacity retention of 91.17%after 800 cycles at 0.5 C.This work provides a facile and accessible approach to manufacturing poly-methyl methacrylate-based polymerization-derived polymer electrolyte and shows great potential as an interphase in Li metal batteries.展开更多
A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel...A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel cell-related electrochemical reactions,their ever-increasing price considerably hinders their industrial application.Improvement of atom utilization efficiency is considered one of the most effective strategies to improve the mass activity of catalysts,and this allows for the use of fewer catalysts,saving greatly on the cost.Thus,single-atom catalysts(SACs)with an atom utilization efficiency of 100%have been widely developed,which show remarkable performance in fuel cells.In this review,we will describe recent progress on the development of SACs for membrane electrode assembly of fuel cell applications.First,we will introduce several effective routes for the synthesis of SACs.The reaction mechanism of the involved reactions will also be introduced as it is highly determinant of the final activity.Then,we will systematically summarize the application of Pt group metal(PGM)and nonprecious group metal(non-PGM)catalysts in membrane electrode assembly of fuel cells.This review will offer numerous experiences for developing potential industrialized fuel cell catalysts in the future.展开更多
The article mainly explores the Hopf bifurcation of a kind of nonlinear system with Gaussian white noise excitation and bounded random parameter.Firstly,the nonlinear system with multisource stochastic fac-tors is red...The article mainly explores the Hopf bifurcation of a kind of nonlinear system with Gaussian white noise excitation and bounded random parameter.Firstly,the nonlinear system with multisource stochastic fac-tors is reduced to an equivalent deterministic nonlinear system by the sequential orthogonal decomposi-tion method and the Karhunen-Loeve(K-L)decomposition theory.Secondly,the critical conditions about the Hopf bifurcation of the equivalent deterministic system are obtained.At the same time the influence of multisource stochastic factors on the Hopf bifurcation for the proposed system is explored.Finally,the theorical results are verified by the numerical simulations.展开更多
The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon m...The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.展开更多
The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we develop...The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors(NASICON)Na_(1.3+x)Al_(0.3)Ce_(x)Ti_(1.7-x)(PO_(4))_(3)(NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide(LiTFSI) matrix.A strong interaction between Ce^(3+)from NCATP and TFSI-anion from the polymer matrix contributes to the fast Li+transportation at the interface.The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0^(-3) S cm^(-1) and a Li^(+) transference number of 0.88.A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm^(-2) presents outstanding cycling stability over 2000 h at 25℃.The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO_(4) at 2 C after 400 cycles and Li/CPEs/LiCoO_(2) at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g^(-1) at 25℃,respectively.展开更多
Graphite tailings produced by natural graphite is usually regarded as garbage to be buried underground,which would result in a certain waste of resources.Here,in order to explore the utilization of natural graphite ta...Graphite tailings produced by natural graphite is usually regarded as garbage to be buried underground,which would result in a certain waste of resources.Here,in order to explore the utilization of natural graphite tailings(NGT),a liquid-polyacrylonitrile(LPAN)is used to modify the NGT fragments and aggregate them together to form secondary graphite particles with low surface area and high tap density.Moreover,the modified NGT show much better electrochemical performances than those of original one.When tested in full cells coupled with NMC532 cathode,the material achieves a high rate capability and cycle stability at the cutoff voltage of 4.25 V as well as 4.45 V,which maintains 84.32%capacity retention after 500 cycles at 1 C rate(4.25 V),higher than that of the pristine one(73.65%).The enhanced performances can be attributed to the use of LPAN to create a unique carbon layer upon graphite tailings to reconstruct surface and repair defects,and also to granulate an isotropic structure of secondary graphite particles,which can help to weaken the anisotropy of Li^(+)diffusion pathway and form a uniform,complete and stable solid-electrolyte-interface(SEI)on the surface of primary NGT fragments to promote a fast Li+diffusion and suppress lithium metal dendrites upon charge and discharge.展开更多
Hypoxic tumor microenvironment is a major challenge for photodynamic therapy(PDT). To overcome this problem, PDT combined hypoxia-activated chemotherapy is a promising strategy for hypoxic cancer therapy. Herein, a mu...Hypoxic tumor microenvironment is a major challenge for photodynamic therapy(PDT). To overcome this problem, PDT combined hypoxia-activated chemotherapy is a promising strategy for hypoxic cancer therapy. Herein, a multifunctional liposome(AQ4N-Ir1-sorafenib-liposome) is prepared by encapsulating a hypoxia-activated prodrug AQ4N, a photosensitizer iridium(III) complex and hepatocellular carcinoma(HCC) targeting drug sorafenib, for synergistic therapy of HCC. Ir1-mediated PDT upon irradiation induces ROS generation and hypoxic environment, which leads to the disassembly of the liposome and activates the antitumor activity of AQ4N. Meantime, the co-delivered sorafenib could effectively target therapy of HCC. It is noted that ferroptosis mechanism is proved during the treatment. This work contributes to the design of hypoxia-responsive multifunctional liposome for combination of chemotherapy, targeting therapy and PDT. It is a promising strategy for hypoxic HCC therapy.展开更多
In this study,dual-metal atomic pairs of manganese(Mn)-iron(Fe)binuclear sites(BNSs)with two conjoint MnN4 and FeN4 moieties(MnFeN8)anchored onto a graphite-like structure(GLS)(Mn-Fe BNSs/GLS)were constructed.The binu...In this study,dual-metal atomic pairs of manganese(Mn)-iron(Fe)binuclear sites(BNSs)with two conjoint MnN4 and FeN4 moieties(MnFeN8)anchored onto a graphite-like structure(GLS)(Mn-Fe BNSs/GLS)were constructed.The binuclear MnFeN8 structure was verified experimentally and theoretically.Magnetic measurements and Gaussian calculations reveal that this unique Mn-Fe BNSs exhibit strong short-range electronic interaction between Mn and Fe sites,which decouples two paired d electrons in Fe sites,thereby transforming Fe sites from an intermediate to a high spin state.The optimal electronic configuration of Fe sites and their binuclear structure facilitate an oxygen reduction reaction(ORR)thermodynamically and dynamically,respectively,endowing Mn-Fe BNSs with improved ORR performance.展开更多
In this study,the morphological distribution of Ru on nitrogen-doped graphene(NG)could be rationally regulated via modulating the combination mode between Ru precursor and the zeolite imidazolate framework-8(ZIF-8).Th...In this study,the morphological distribution of Ru on nitrogen-doped graphene(NG)could be rationally regulated via modulating the combination mode between Ru precursor and the zeolite imidazolate framework-8(ZIF-8).The cation exchange and host-guest strategies respectively resulted in two different combination modes between Ru precursor and ZIF-8 anchored on graphene.Following pyrolysis of the above precursors,Ru single-atom sites(SASs)with and without Ru nanoparticles(NPs)were formed selectively on NG(denoted as Ru SASs+NPs/NG and Ru SASs/NG,respectively).Ru SASs+NPs/NG exhibited excellent hydrogen evolution reaction(HER)performance in alkaline solutions(η_(10)=12 mV,12.57 A mg^(-1)_(Ru) at 100 mV),which is much better than Ru SASs/NG.The experimental and theoretical study revealed that Ru SASs could adsorb hydrogen with optimal adsorption strength,while Ru NPs could lower the barrier of water molecule dissociation,and thus Ru SASs and Ru NPs could synergistically promote the catalytic performance of HER in alkaline solutions.展开更多
Metal-based compounds with excellent photo-physical properties show good photochemotherapeutic performance.But,low in-depth tissue penetration of light limits their effectivity for deeply buried tumors.Encouraged by t...Metal-based compounds with excellent photo-physical properties show good photochemotherapeutic performance.But,low in-depth tissue penetration of light limits their effectivity for deeply buried tumors.Encouraged by the sonosensitizing ability of the traditional organic photosensitizers,here,we developed AuNPs@Ir1 as a sonosensitizer by hybridizing an organometallic Ir(Ⅲ) complex(Ir1) with ultrasmall gold nanoparticles(AuNPs) for efficient tumor sonodynamic therapy(SDT) for the first time.AuNPs@Ir1 rapidly entered the cancer cells,produced ^(1)O_(2),and catalytically oxidized NADH to NAD;under ultrasound(US)irradiation,thus resulted in cancer cells oncosis.Because of efficient passive retention in tumors post intravenous injection,AuNPs@Ir1 further efficiently inhibited the growth of tumors in-vivo under US stimulation without long-term toxicity to other organs.Overall,this work presents the excellent US triggered in-vitro and in-vivo anticancer profile of the novel AuNPs@Ir1.It is expected to increase the scope of SDT for metal-based anticancer drugs.展开更多
基金financial support by National Natural Science Foundation(NNSF)of China(Nos.52202269,52002248,U23B2069,22309162)Shenzhen Science and Technology program(No.20220810155330003)+1 种基金Shenzhen Basic Research Project(No.JCYJ20190808163005631)Xiangjiang Lab(22XJ01007).
文摘Sodium-ion batteries hold great promise as next-generation energy storage systems.However,the high instability of the electrode/electrolyte interphase during cycling has seriously hindered the development of SIBs.In particular,an unstable cathode–electrolyte interphase(CEI)leads to successive electrolyte side reactions,transition metal leaching and rapid capacity decay,which tends to be exacerbated under high-voltage conditions.Therefore,constructing dense and stable CEIs are crucial for high-performance SIBs.This work reports localized high-concentration electrolyte by incorporating a highly oxidation-resistant sulfolane solvent with non-solvent diluent 1H,1H,5H-octafluoropentyl-1,1,2,2-tetrafluoroethyl ether,which exhibited excellent oxidative stability and was able to form thin,dense and homogeneous CEI.The excellent CEI enabled the O3-type layered oxide cathode NaNi_(1/3)Mn_(1/3)Fe_(1/3)O_(2)(NaNMF)to achieve stable cycling,with a capacity retention of 79.48%after 300 cycles at 1 C and 81.15%after 400 cycles at 2 C with a high charging voltage of 4.2 V.In addition,its nonflammable nature enhances the safety of SIBs.This work provides a viable pathway for the application of sulfolane-based electrolytes on SIBs and the design of next-generation high-voltage electrolytes.
基金supported by the National Natural Science Foundation of China(22109100,22075203)Guangdong Basic and Applied Basic Research Foundation(2022A1515011677)+1 种基金Shenzhen Science and Technology Project Program(JCYJ2021032409420401)Natural Science Foundation of SZU(000002111605).
文摘The high-temperature pyrolysis process for preparing M–N–C single-atom catalyst usually results in high heterogeneity in product structure concurrently contains multiscale metal phases from single atoms(SAs),atomic clusters to nanoparticles.Therefore,understanding the interactions among these components,especially the synergistic effects between single atomic sites and cluster sites,is crucial for improving the oxygen reduction reaction(ORR)activity of M–N–C catalysts.Accordingly,herein,we constructed a model catalyst composed of both atomically dispersed FeN4 SA sites and adjacent Fe clusters through a site occupation strategy.We found that the Fe clusters can optimize the adsorption strength of oxygen reduction intermediates on FeN4 SA sites by introducing electron-withdrawing–OH ligands and decreasing the d-band center of the Fe center.The as-developed catalyst exhibits encouraging ORR activity with halfwave potentials(E1/2)of 0.831 and 0.905 V in acidic and alkaline media,respectively.Moreover,the catalyst also represents excellent durability exceeding that of Fe–N–C SA catalyst.The practical application of Fe(Cd)–CNx catalyst is further validated by its superior activity and stability in a metalair battery device.Our work exhibits the great potential of synergistic effects between multiphase metal species for improvements of singleatom site catalysts.
基金funded by the National Key Research and Development Program of China(no.2020YFC1909604)Shenzhen Key Projects of Technological Research(JSGG20200925145800001)Shenzhen Basic Research Project(no.JCYJ20190808145203535).
文摘This work demonstrates a novel polymerization-derived polymer electrolyte consisting of methyl methacrylate,lithium bis(trifluoromethanesulfonyl)imide and fluoroethylene carbonate.The polymerization of MMA was initiated by the amino compounds following an anionic catalytic mechanism.LiTFSI plays both roles including the initiator and Li ion source in the polymer electrolyte.Normally,lithium bis(trifluoromethanesulfonyl)imide has difficulty in initiating the polymerization reaction of methyl methacrylate monomer,a very high concentration of lithium bis(trifluoromethanesulfonyl)imide is needed for initiating the polymerization.However,the fluoroethylene carbonate additive can work as a supporter to facilitate the degree of dissociation of lithium bis(trifluoromethanesulfonyl)imide and increase its initiator capacity due to the high dielectric constant.The as-prepared poly-methyl methacrylate-based polymer electrolyte has a high ionic conductivity(1.19×10^(−3)S cm^(−1)),a wide electrochemical stability window(5 V vs Li^(+)/Li),and a high Li ion transference number(t_(Li^(+)))of 0.74 at room temperature(RT).Moreover,this polymerization-derived polymer electrolyte can effectively work as an artificial protective layer on Li metal anode,which enabled the Li symmetric cell to achieve a long-term cycling performance at 0.2 mAh cm^(−2)for 2800 h.The LiFePO_(4)battery with polymerization-derived polymer electrolyte-modified Li metal anode shows a capacity retention of 91.17%after 800 cycles at 0.5 C.This work provides a facile and accessible approach to manufacturing poly-methyl methacrylate-based polymerization-derived polymer electrolyte and shows great potential as an interphase in Li metal batteries.
基金National Natural Science Foundation of China,Grant/Award Numbers:22075203,22279079,21905179Guangdong Science and Technology Department Program,Grant/Award Number:2021QN02L252+1 种基金Shenzhen Science and Technology Department Program,Grant/Award Numbers:20220810133521001,20220809165014001Natural Science Foundation of SZU,Grant/Award Numbers:000002111605,000002112215。
文摘A fuel cell is an energy conversion device that can continuously input fuel and oxidant into the device through an electrochemical reaction to release electrical energy.Although noble metals show good activity in fuel cell-related electrochemical reactions,their ever-increasing price considerably hinders their industrial application.Improvement of atom utilization efficiency is considered one of the most effective strategies to improve the mass activity of catalysts,and this allows for the use of fewer catalysts,saving greatly on the cost.Thus,single-atom catalysts(SACs)with an atom utilization efficiency of 100%have been widely developed,which show remarkable performance in fuel cells.In this review,we will describe recent progress on the development of SACs for membrane electrode assembly of fuel cell applications.First,we will introduce several effective routes for the synthesis of SACs.The reaction mechanism of the involved reactions will also be introduced as it is highly determinant of the final activity.Then,we will systematically summarize the application of Pt group metal(PGM)and nonprecious group metal(non-PGM)catalysts in membrane electrode assembly of fuel cells.This review will offer numerous experiences for developing potential industrialized fuel cell catalysts in the future.
基金This work was supported by the grants from the National Nat-ural Science Foundation of China(No.11772002)Ningxia higher education first-class discipline construction funding project(No.NXYLXK2017B09)+2 种基金Major Special project of North Minzu University(No.ZDZX201902)Open project of The Key Laboratory of In-telligent Information and Big Data Processing of NingXia Province(No.2019KLBD008)Postgraduate Innovation Project of North Minzu University(No.YCX22099).
文摘The article mainly explores the Hopf bifurcation of a kind of nonlinear system with Gaussian white noise excitation and bounded random parameter.Firstly,the nonlinear system with multisource stochastic fac-tors is reduced to an equivalent deterministic nonlinear system by the sequential orthogonal decomposi-tion method and the Karhunen-Loeve(K-L)decomposition theory.Secondly,the critical conditions about the Hopf bifurcation of the equivalent deterministic system are obtained.At the same time the influence of multisource stochastic factors on the Hopf bifurcation for the proposed system is explored.Finally,the theorical results are verified by the numerical simulations.
文摘The electrochemical reduction of CO2(CO2 RR) can substantially contribute to the production of useful chemicals and reduction of global CO2 emissions. Herein, we presented N and S dual-doped high-surface-area carbon materials(SZ-HCN) as CO2 RR catalysts. N and S were doped by one-step pyrolysis of a N-containing polymer and S powder. ZnCl2 was applied as a volatile porogen to prepare porous SZ-HCN. SZ-HCN with a high specific surface area(1510 m2 g–1) exhibited efficient electrocatalytic activity and selectivity for CO2 RR. Electrochemical measurements demonstrated that SZ-HCN showed excellent catalytic performance for CO2-to-CO reduction with a high CO Faradaic efficiency(~93%) at-0.6 V. Furthermore, SZ-HCN offered a stable current density and high CO selectivity over at least 20 h continuous operation, revealing remarkable electrocatalytic durability. The experimental results and density functional theory calculations indicated that N and S dual-doped carbon materials required lower Gibbs free energy to form the COOH* intermediate than that for single-N-doped carbon for CO2-to-CO reduction, thereby enhancing CO2 RR activity.
基金the National Key Research and Development Program of China (No. 2020YFC1909604)the Shenzhen Key Projects of Technological Research (JSGG2020092514 5800001)。
文摘The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors(NASICON)Na_(1.3+x)Al_(0.3)Ce_(x)Ti_(1.7-x)(PO_(4))_(3)(NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide(LiTFSI) matrix.A strong interaction between Ce^(3+)from NCATP and TFSI-anion from the polymer matrix contributes to the fast Li+transportation at the interface.The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0^(-3) S cm^(-1) and a Li^(+) transference number of 0.88.A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm^(-2) presents outstanding cycling stability over 2000 h at 25℃.The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO_(4) at 2 C after 400 cycles and Li/CPEs/LiCoO_(2) at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g^(-1) at 25℃,respectively.
基金the financial support of National Key Research and Development Program of China(No.2020YFC1909604)National Natural Science Foundation(NNSF)of China(Nos.52202269,52002248)+1 种基金Shenzhen Key Projects of Technological Research(No.JSGG20200925145800001)and Shenzhen Basic Research Project(Nos.JCYJ20190808145203535,JCYJ20190808163005631)for providing financial support for this work.We are also grateful to the Instrumental Analysis Center of Shenzhen University(Xili Campus)for providing the facilities for our material analyzes。
文摘Graphite tailings produced by natural graphite is usually regarded as garbage to be buried underground,which would result in a certain waste of resources.Here,in order to explore the utilization of natural graphite tailings(NGT),a liquid-polyacrylonitrile(LPAN)is used to modify the NGT fragments and aggregate them together to form secondary graphite particles with low surface area and high tap density.Moreover,the modified NGT show much better electrochemical performances than those of original one.When tested in full cells coupled with NMC532 cathode,the material achieves a high rate capability and cycle stability at the cutoff voltage of 4.25 V as well as 4.45 V,which maintains 84.32%capacity retention after 500 cycles at 1 C rate(4.25 V),higher than that of the pristine one(73.65%).The enhanced performances can be attributed to the use of LPAN to create a unique carbon layer upon graphite tailings to reconstruct surface and repair defects,and also to granulate an isotropic structure of secondary graphite particles,which can help to weaken the anisotropy of Li^(+)diffusion pathway and form a uniform,complete and stable solid-electrolyte-interface(SEI)on the surface of primary NGT fragments to promote a fast Li+diffusion and suppress lithium metal dendrites upon charge and discharge.
基金financially supported by the National Natural Science Foundation of China(11921006)the National Key Research and Development Program of China(2020YFC1909604)+1 种基金Shenzhen Key Projects of Technological Research(JSGG20200925145800001)Shenzhen Science and Technology Program(CJGJZD20210408092801005)。
基金the financial support of the National Natural Science Foundation of China (NSFC, Nos. 22077085, 22007104,22177078, 21907069)the Project of the Natural Science Foundation of Guangdong Province (No. 2019A1515011958)the Science and Technology Foundation of Shenzhen (Nos.JCYJ20210324095200002 and JCYJ20190808153209537)。
文摘Hypoxic tumor microenvironment is a major challenge for photodynamic therapy(PDT). To overcome this problem, PDT combined hypoxia-activated chemotherapy is a promising strategy for hypoxic cancer therapy. Herein, a multifunctional liposome(AQ4N-Ir1-sorafenib-liposome) is prepared by encapsulating a hypoxia-activated prodrug AQ4N, a photosensitizer iridium(III) complex and hepatocellular carcinoma(HCC) targeting drug sorafenib, for synergistic therapy of HCC. Ir1-mediated PDT upon irradiation induces ROS generation and hypoxic environment, which leads to the disassembly of the liposome and activates the antitumor activity of AQ4N. Meantime, the co-delivered sorafenib could effectively target therapy of HCC. It is noted that ferroptosis mechanism is proved during the treatment. This work contributes to the design of hypoxia-responsive multifunctional liposome for combination of chemotherapy, targeting therapy and PDT. It is a promising strategy for hypoxic HCC therapy.
基金support of Shenzhen Basic Research Project(Nos.JCYJ20170818092720054,JCYJ20190808145203535,and JCYJ20190808144413257)National Natural Science Foundation of China(No.21671136)+3 种基金Postdoctoral Science Foundation of China(No.2019M663085)Major Programs for Science and Technology Development of Shenzhen(Nos.JSGG20160328151657828 and XCL201110060)Major Industrial Projects of Shenzhen(No.s2017001850011)the Project of Natural Science Foundation of Guangdong Province(Nos.2020A1515010380 and 2014A030311028).
文摘In this study,dual-metal atomic pairs of manganese(Mn)-iron(Fe)binuclear sites(BNSs)with two conjoint MnN4 and FeN4 moieties(MnFeN8)anchored onto a graphite-like structure(GLS)(Mn-Fe BNSs/GLS)were constructed.The binuclear MnFeN8 structure was verified experimentally and theoretically.Magnetic measurements and Gaussian calculations reveal that this unique Mn-Fe BNSs exhibit strong short-range electronic interaction between Mn and Fe sites,which decouples two paired d electrons in Fe sites,thereby transforming Fe sites from an intermediate to a high spin state.The optimal electronic configuration of Fe sites and their binuclear structure facilitate an oxygen reduction reaction(ORR)thermodynamically and dynamically,respectively,endowing Mn-Fe BNSs with improved ORR performance.
基金supported by the National Key Research and Development Program of China(2020YFC1909604)Shenzhen Key Projects of Technological Research(JSGG20200925145800001)+1 种基金Shenzhen Basic Research Project(JCYJ20190808145203535,JCYJ20190808144413257)the Project of Natural Science Foundation of Guangdong Province(2020A1515010379)。
文摘In this study,the morphological distribution of Ru on nitrogen-doped graphene(NG)could be rationally regulated via modulating the combination mode between Ru precursor and the zeolite imidazolate framework-8(ZIF-8).The cation exchange and host-guest strategies respectively resulted in two different combination modes between Ru precursor and ZIF-8 anchored on graphene.Following pyrolysis of the above precursors,Ru single-atom sites(SASs)with and without Ru nanoparticles(NPs)were formed selectively on NG(denoted as Ru SASs+NPs/NG and Ru SASs/NG,respectively).Ru SASs+NPs/NG exhibited excellent hydrogen evolution reaction(HER)performance in alkaline solutions(η_(10)=12 mV,12.57 A mg^(-1)_(Ru) at 100 mV),which is much better than Ru SASs/NG.The experimental and theoretical study revealed that Ru SASs could adsorb hydrogen with optimal adsorption strength,while Ru NPs could lower the barrier of water molecule dissociation,and thus Ru SASs and Ru NPs could synergistically promote the catalytic performance of HER in alkaline solutions.
基金financial support of the National Natural Science Foundation of China (NSFC, Nos. 22077085, 22007104)the Project of the Natural Science Foundation of Guangdong Province(No. 2019A1515011958)+2 种基金the Science and Technology Foundation of Shenzhen (No. JCYJ20190808153209537)DST,the Government of India (No. DST/INSPIRE/04/2019/000492)the Instrumental Analysis Center of Shenzhen University。
文摘Metal-based compounds with excellent photo-physical properties show good photochemotherapeutic performance.But,low in-depth tissue penetration of light limits their effectivity for deeply buried tumors.Encouraged by the sonosensitizing ability of the traditional organic photosensitizers,here,we developed AuNPs@Ir1 as a sonosensitizer by hybridizing an organometallic Ir(Ⅲ) complex(Ir1) with ultrasmall gold nanoparticles(AuNPs) for efficient tumor sonodynamic therapy(SDT) for the first time.AuNPs@Ir1 rapidly entered the cancer cells,produced ^(1)O_(2),and catalytically oxidized NADH to NAD;under ultrasound(US)irradiation,thus resulted in cancer cells oncosis.Because of efficient passive retention in tumors post intravenous injection,AuNPs@Ir1 further efficiently inhibited the growth of tumors in-vivo under US stimulation without long-term toxicity to other organs.Overall,this work presents the excellent US triggered in-vitro and in-vivo anticancer profile of the novel AuNPs@Ir1.It is expected to increase the scope of SDT for metal-based anticancer drugs.
