High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion te...High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.展开更多
The selective hydrogenolysis of glycerol exhibits great prospects,while the catalysts with high selectivity and activity are still missing and need to be created urgently.Herein,we report the synthesis of hollow mesop...The selective hydrogenolysis of glycerol exhibits great prospects,while the catalysts with high selectivity and activity are still missing and need to be created urgently.Herein,we report the synthesis of hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)nanosphere catalysts with bi-functional interfaces synergistically for high efficiency conversion of glycerol to 1,3-propanediol.The hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)catalysts show a typical brick-concrete liked framework with a high surface area(179.3 m^(2)·g^(-1)),large mesopore size(10.6 nm),uniform particle size(~400 nm),and ultrathin shell thickness(~75 nm).The brick anatase nanocrystals and concrete amorphous SiO_(2)networks can selectively rivet Pt nanoparticles and WO_(x)nanocluster species,respectively,thus constructing two interfaces for effective adsorption,rapidly catalytic dehydration and hydrogenation processes.The hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)catalysts deliver a high selectivity of 53.8%for 1,3-propanediol(1,3-PDO)at a very high glycerol conversion of 85.0%.As a result,a favorable 1,3-PDO yield of 45.7%can be obtained with excellent stability,which is among the best performances of previously reported catalysts.This work paves a new way to synthesize catalysts with high selectivity,high activity and high stability.展开更多
Lowering the operating temperature of solid oxide fuel cells(SOFCs)has extensively stimulated the development of new oxide ion conductors.Here,inspired by the structural commonalities of oxide ion conductors,the inabi...Lowering the operating temperature of solid oxide fuel cells(SOFCs)has extensively stimulated the development of new oxide ion conductors.Here,inspired by the structural commonalities of oxide ion conductors,the inability to accommodate oxygen vacancies in the rigid,isolated,3-fold tetrahedral rings of SrSi/GeO_(3)-based materials,and the considerable flexibility of BO_(n) polyhedra in terms of coordination number,rotation,deformation,and linkage,we report the first borate-base family of oxide ion conductors,(Gd/Y)_(1−x)Zn_(x)BO_(3−0.5x),through combined computational prediction and experimental verification.The oxygen vacancies in(Gd/Y)BO_(3)can be accommodated by forming B_(3)O_(8)units in isolated,3-fold,tetrahedral rings of B_(3)O_(9)and transported through a cooperative mechanism of oxygen exchange between the B_(3)O_(9)and B_(3)O_(8)units,which is assisted by the intermediate opening and extending of these units.This study opens a new scientific field of the borate system for designing and discovering oxide ion conductors.展开更多
In the version of the article originally published in the volume 62,issue 10,2022 of Sci.china Mater.(page 2737-2745,https://doi.org/10.1007/s40843-022-2044-3).The chemical shift reported in Figure 5f for the^(11)B so...In the version of the article originally published in the volume 62,issue 10,2022 of Sci.china Mater.(page 2737-2745,https://doi.org/10.1007/s40843-022-2044-3).The chemical shift reported in Figure 5f for the^(11)B solid-state NMR spectra is incorrect because no parameter correction was performed during data processing.展开更多
基金the staff at Beamline (BL08U1-A and BL11B)of the Shanghai Synchrotron Radiation Facility (SSRF)the support from the National Key Research&Development Program of China (2022YFB3803700)+2 种基金the National Natural Science Foundation of China (52171186)the support through the Overseas Outstanding Youth Fund and Shanghai Pujiang Talent Project (21PJ1408500)the financial support from the Center of Hydrogen Science,Shanghai Jiao Tong University。
文摘High efficiency,cost-effective and durable electrocatalysts are of pivotal importance in energy conversion and storage systems.The electro-oxidation of water to oxygen plays a crucial role in such energy conversion technologies.Herein,we report a robust method for the synthesis of a bimetallic alkoxide for efficient oxygen evolution reaction(OER)for alkaline electrolysis,which yields current density of 10 mA cm^(-2)at an overpotential of 215 mV in 0.1 M KOH electrolyte.The catalyst demonstrates an excellent durability for more than 540 h operation with negligible degradation in activity.Raman spectra revealed that the catalyst underwent structure reconstruction during OER,evolving into oxyhydroxide,which was the active site proceeding OER in alkaline electrolyte.In-situ synchrotron X-ray absorption experiment combined with density functional theory calculation suggests a lattice oxygen involved electrocatalytic reaction mechanism for the in-situ generated nickel–iron bimetal-oxyhydroxide catalyst.This mechanism together with the synergy between nickel and iron are responsible for the enhanced catalytic activity and durability.These findings provide promising strategies for the rational design of nonnoble metal OER catalysts.
基金This work was supported by the National Key R&D Program of China(Nos.2022YFA1503501 and 2018YFA0209401)the National Natural Science Foundation of China(Nos.22088101,21975050 and U21A20329)+2 种基金the Program of Shanghai Academic Research Leader(No.21XD1420800)the Shanghai Pilot Program for Basic Research-Fudan University 21TQ1400100(No.21TQ008)the Fundamental Research Funds for the Central Universities(No.20720220010).
文摘The selective hydrogenolysis of glycerol exhibits great prospects,while the catalysts with high selectivity and activity are still missing and need to be created urgently.Herein,we report the synthesis of hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)nanosphere catalysts with bi-functional interfaces synergistically for high efficiency conversion of glycerol to 1,3-propanediol.The hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)catalysts show a typical brick-concrete liked framework with a high surface area(179.3 m^(2)·g^(-1)),large mesopore size(10.6 nm),uniform particle size(~400 nm),and ultrathin shell thickness(~75 nm).The brick anatase nanocrystals and concrete amorphous SiO_(2)networks can selectively rivet Pt nanoparticles and WO_(x)nanocluster species,respectively,thus constructing two interfaces for effective adsorption,rapidly catalytic dehydration and hydrogenation processes.The hollow mesoporous Pt/WO_(x)/SiO_(2)-TiO_(2)catalysts deliver a high selectivity of 53.8%for 1,3-propanediol(1,3-PDO)at a very high glycerol conversion of 85.0%.As a result,a favorable 1,3-PDO yield of 45.7%can be obtained with excellent stability,which is among the best performances of previously reported catalysts.This work paves a new way to synthesize catalysts with high selectivity,high activity and high stability.
基金the National Natural Science Foundation of China(22090043 and 21622101)Guangxi Natural Science Foundation(2019GXNSFGA245006)for financial support+2 种基金the National Natural Science Foundation of China(21527803 and 21621061)the Ministry of Science and Technology of China(2016YFA0301004)for financial supportthe funding from China Postdoctoral Science Foundation(8206300392)。
文摘Lowering the operating temperature of solid oxide fuel cells(SOFCs)has extensively stimulated the development of new oxide ion conductors.Here,inspired by the structural commonalities of oxide ion conductors,the inability to accommodate oxygen vacancies in the rigid,isolated,3-fold tetrahedral rings of SrSi/GeO_(3)-based materials,and the considerable flexibility of BO_(n) polyhedra in terms of coordination number,rotation,deformation,and linkage,we report the first borate-base family of oxide ion conductors,(Gd/Y)_(1−x)Zn_(x)BO_(3−0.5x),through combined computational prediction and experimental verification.The oxygen vacancies in(Gd/Y)BO_(3)can be accommodated by forming B_(3)O_(8)units in isolated,3-fold,tetrahedral rings of B_(3)O_(9)and transported through a cooperative mechanism of oxygen exchange between the B_(3)O_(9)and B_(3)O_(8)units,which is assisted by the intermediate opening and extending of these units.This study opens a new scientific field of the borate system for designing and discovering oxide ion conductors.
文摘In the version of the article originally published in the volume 62,issue 10,2022 of Sci.china Mater.(page 2737-2745,https://doi.org/10.1007/s40843-022-2044-3).The chemical shift reported in Figure 5f for the^(11)B solid-state NMR spectra is incorrect because no parameter correction was performed during data processing.