The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-dop...The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In2.77S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2)production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In2.77S_(4),respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In2.77S_(4)according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2)production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2)around the active centers,the energy barriers of O_(2)protonation and H_(2)O_(2)desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2)photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.展开更多
Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and on...Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and only a limited candidates have been reported so far.In this work,we found for the first time that a continuous solid solution,Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2)(0≤α≤1,could be obtained by mutual substitution of cations at center‐symmetric Na3 and Na4 sites while keeping the crystal building blocks of anionic P_(2)O_(7) unchanged.In particular,a novel off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)is thus proposed,and its structure,energy storage mechanism,and electrochemical performance are extensively investigated to unveil the structure–function relationship.The as‐prepared off‐stoichiometric electrode delivers appealing performance with a reversible discharge capacity of 83 mAh g^(−1),a working voltage of 2.9 V(vs.Na^(+)/Na),the retention of 89.2%of the initial capacity after 500 cycles,and enhanced rate capability of 51 mAh g^(−1)at a current density of 1600 mA g^(−1).This research shows that sodium ferric pyrophosphate could form extended solid solution composition and promising phase is concealed in the range of Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2),offering more chances for exploration of new cathode materials for the construction of high‐performance SIBs.展开更多
WC-10Co cemented carbides with finer WC and narrower grain size distributions are produced by using(Cr,V)_(2)(C,N)as grain growth inhibitors.As a result,with the increase of(Cr_(0.9),V_(0.1))_(2)(C,N)and(V_(0.9),Cr_(0...WC-10Co cemented carbides with finer WC and narrower grain size distributions are produced by using(Cr,V)_(2)(C,N)as grain growth inhibitors.As a result,with the increase of(Cr_(0.9),V_(0.1))_(2)(C,N)and(V_(0.9),Cr_(0.1))_(2)(C,N),the grains size of WC and mean free path of Co phase decrease,and adjacency of WC increases.Refinement and homogenization of grains enhance the transverse rupture strength(TRS)and the hardness.Meanwhile,the deflection and bridging of cracks keep the fracture toughness at a respectable level.The WC-10Co-0.6(Cr_(0.9),V_(0.1))_(2)(C,N)-0.025(V_(0.9),Cr_(0.1))_(2)(C,N)cemented carbides exhibit excellent comprehensive mechanical properties with the TRS of 4602.6 MPa,hardness of 1835 kg/mm^(2),and fracture toughness of 10.39 MPa·m^(1/2),respectively.However,the large pores are caused by excess N larger than 0.03 wt%and deteriorates the mechanical properties.We provide a new approach to WC-Co cemented carbides preparation with a narrow grain size distribution by adding novel grain growth inhibitors.展开更多
由公式C<sub>n</sub><sup>k</sup>+C<sub>n</sub><sup>k+1</sup>=C<sub>n+1</sub><sup>k+1</sup>,可得:C<sub>2</sub><sup>2</sup>+...由公式C<sub>n</sub><sup>k</sup>+C<sub>n</sub><sup>k+1</sup>=C<sub>n+1</sub><sup>k+1</sup>,可得:C<sub>2</sub><sup>2</sup>+C<sub>3</sub><sup>2</sup>+…+C<sub>n</sub><sup>2</sup>=C<sub>n+1</sub><sup>3</sup>,sum from k=2 to nC<sub>k</sub><sup>2</sup>=C<sub>n+1</sub><sup>3</sup>,展开更多
文摘The development of an efficient artificial H_(2)O_(2)photosynthesis system is a challenging work using H_(2)O and O_(2)as starting materials.Herein,3D In2.77S_(4)nanoflower precursor was in-situ deposited on K^(+)-doped g-C_(3)N_(4)(KCN)nanosheets using a solvothermal method,then In2.77S_(4)/KCN(IS/KCN)het-erojunction with an intimate interface was obtained after a calcination process.The investigation shows that the photocatalytic H_(2)O_(2)production rate of 50IS/KCN can reach up to 1.36 mmol g^(-1)h^(-1)without any sacrificial reagents under visible light irradiation,which is 9.2 times and 4.1 times higher than that of KCN and In2.77S_(4),respectively.The enhanced activity of the above composite can be mainly attributed to the S-scheme charge transfer route between KCN and In2.77S_(4)according to density functional theory calculations,electron paramagnetic resonance and free radical capture tests,leading to an expanded light response range and rapid charge separation at their interface,as well as preserving the active electrons and holes for H_(2)O_(2)production.Besides,the unique 3D nanostructure and surface hydrophobicity of IS/KCN facilitate the diffusion and transportation of O_(2)around the active centers,the energy barriers of O_(2)protonation and H_(2)O_(2)desorption steps are ef-fectively reduced over the composite.In addition,this system also exhibits excellent light harvesting ability and stability.This work provides a potential strategy to explore a sustainable H_(2)O_(2)photo-synthesis pathway through the design of heterojunctions with intimate interfaces and desired reac-tion thermodynamics and kinetics.
基金National Natural Science Foundation of China,Grant/Award Numbers:21972108,U20A20249,U22A20438Changzhou Science and Technology Bureau,Grant/Award Number:CM20223017Innovation and Technology Commission(ITC)of Hong Kong,The Innovation&Technology Fund(ITF)with Project No.ITS/126/21。
文摘Iron‐based pyrophosphates are attractive cathodes for sodium‐ion batteries due to their large framework,cost‐effectiveness,and high energy density.However,the understanding of the crystal structure is scarce and only a limited candidates have been reported so far.In this work,we found for the first time that a continuous solid solution,Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2)(0≤α≤1,could be obtained by mutual substitution of cations at center‐symmetric Na3 and Na4 sites while keeping the crystal building blocks of anionic P_(2)O_(7) unchanged.In particular,a novel off‐stoichiometric Na_(3)Fe(2.5)(P_(2)O_(7))_(2)is thus proposed,and its structure,energy storage mechanism,and electrochemical performance are extensively investigated to unveil the structure–function relationship.The as‐prepared off‐stoichiometric electrode delivers appealing performance with a reversible discharge capacity of 83 mAh g^(−1),a working voltage of 2.9 V(vs.Na^(+)/Na),the retention of 89.2%of the initial capacity after 500 cycles,and enhanced rate capability of 51 mAh g^(−1)at a current density of 1600 mA g^(−1).This research shows that sodium ferric pyrophosphate could form extended solid solution composition and promising phase is concealed in the range of Na_(4−α)Fe_(2+α)_(2)(P_(2)O_(7))_(2),offering more chances for exploration of new cathode materials for the construction of high‐performance SIBs.
基金This work is supported by the National Natural Science Foundation of China(No.22103075,No.21827804,and No.22173089)the National Key R&D Program of China(No.2021YFA0716801andNo.2017YFA0303502).
基金Funded by the 2021 Strategic Cooperation Project between Sichuan University and The People's Government of Zigong(No.2021CDZG-1)Major Science and Technology Research Projects of Panxi,Sichuan Province(No.2022PXZB-04)。
文摘WC-10Co cemented carbides with finer WC and narrower grain size distributions are produced by using(Cr,V)_(2)(C,N)as grain growth inhibitors.As a result,with the increase of(Cr_(0.9),V_(0.1))_(2)(C,N)and(V_(0.9),Cr_(0.1))_(2)(C,N),the grains size of WC and mean free path of Co phase decrease,and adjacency of WC increases.Refinement and homogenization of grains enhance the transverse rupture strength(TRS)and the hardness.Meanwhile,the deflection and bridging of cracks keep the fracture toughness at a respectable level.The WC-10Co-0.6(Cr_(0.9),V_(0.1))_(2)(C,N)-0.025(V_(0.9),Cr_(0.1))_(2)(C,N)cemented carbides exhibit excellent comprehensive mechanical properties with the TRS of 4602.6 MPa,hardness of 1835 kg/mm^(2),and fracture toughness of 10.39 MPa·m^(1/2),respectively.However,the large pores are caused by excess N larger than 0.03 wt%and deteriorates the mechanical properties.We provide a new approach to WC-Co cemented carbides preparation with a narrow grain size distribution by adding novel grain growth inhibitors.
文摘由公式C<sub>n</sub><sup>k</sup>+C<sub>n</sub><sup>k+1</sup>=C<sub>n+1</sub><sup>k+1</sup>,可得:C<sub>2</sub><sup>2</sup>+C<sub>3</sub><sup>2</sup>+…+C<sub>n</sub><sup>2</sup>=C<sub>n+1</sub><sup>3</sup>,sum from k=2 to nC<sub>k</sub><sup>2</sup>=C<sub>n+1</sub><sup>3</sup>,
