Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alyt...Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active sites.Surface chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction pathways.In this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic effect.More importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and perspective.This work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.展开更多
The bone repair niche,including the physiological and pathological microenvironment,is a complex system that interferes with various cellular/noncellular activities.Thus,a rational perspective of designing tunable bio...The bone repair niche,including the physiological and pathological microenvironment,is a complex system that interferes with various cellular/noncellular activities.Thus,a rational perspective of designing tunable biomaterials with the modulation of the bone microenvironment is in high demand in pre/clinical practice for the management of refractory bone defects in combination with severe bone diseases.Two-dimensional(2D)layered materials are emerging biomaterials for bone microenvironment engineering because of their inherent biocompatibility,osteo-inductivity,osteo-conductivity,optical properties,enzyme mimetics,and mechanical properties.In this study,we focus on the latest advances in developing 2D layered materials in bone regeneration,bone cancer therapies,bone-related infections eradication,and articular cartilage repair.In addition,the specific action mechanisms and design regimens of 2D-layered material-based nanoplatforms are clarified.Finally,the current challenges are discussed,and the key inspirations for further broadening the pre/clinical applications of 2D layered materials in orthopedic disorder therapy are proposed.展开更多
Engineering of enzyme microenvironment can surprisingly boost the apparent activity.However,the underlying regulation mechanism is not well-studied at a molecular level so far.Here,we present a modulation of two model...Engineering of enzyme microenvironment can surprisingly boost the apparent activity.However,the underlying regulation mechanism is not well-studied at a molecular level so far.Here,we present a modulation of two model enzymes of cytochrome c(Cty C)and D-amino acid oxidase(DAAO)with opposite pH-activity profiles using ionic polymers.The operational pH of poly(acrylic acid)modified Cyt C and polyallylamine modified DAAO was extended to 3-7 and 2-10 where the enzyme activity was larger than that at their optimum pH of 4.5 and 8.5 by 106%and 28%,respectively.The cascade reaction catalyzed by two modified enzymes reveals a 1.37-fold enhancement in catalytic efficiency compared with their native counterparts.The enzyme activity boosting is understood by performing the UV-vis/CD spectroscopy and molecular dynamics simulations in the atomistic level.The increased activity is ascribed to the favorable microenvironment in support of preserving enzyme native structures nearby cofactor under external perturbations.展开更多
基金supported by the Key Research&Development and Promotion Projects in Henan Province(No.232102230079).
文摘Electrocatalysis is a surface-sensitive process,in which the catalytic activity of electrocatalyst highly re-lates to the surface adsorption/desorption behaviors of the reactants/intermediates/products on the cat-alytically active sites.Surface chemical microenvironment engineering via organic molecules functional-ization is a promising strategy to tune the electrocatalytic activity since it can well modify the elec-trode/electrolyte interface and alter the reaction pathways.In this review,we summarize the recent progress of surface microenvironment engineering of electrocatalysts induced by organic molecules func-tionalization,with the special focus on the organic molecule-assisted growth mechanism and unique electronic effect.More importantly,the applications of organic molecule functionalized catalysts in var-ious electrocatalytic reactions are also systematically summarized,along with a deep discussion on the conclusion and perspective.This work will open a new avenue for the construction and modification of advanced electrocatalysts based on organic molecule-mediated interface engineering.
基金the National Natural Science Foundation of China(62174013,92265111,52302343)the funding Program of BIT(3180012212214,3180023012204,RCPT-20220029,XSQD6120220130).
文摘The bone repair niche,including the physiological and pathological microenvironment,is a complex system that interferes with various cellular/noncellular activities.Thus,a rational perspective of designing tunable biomaterials with the modulation of the bone microenvironment is in high demand in pre/clinical practice for the management of refractory bone defects in combination with severe bone diseases.Two-dimensional(2D)layered materials are emerging biomaterials for bone microenvironment engineering because of their inherent biocompatibility,osteo-inductivity,osteo-conductivity,optical properties,enzyme mimetics,and mechanical properties.In this study,we focus on the latest advances in developing 2D layered materials in bone regeneration,bone cancer therapies,bone-related infections eradication,and articular cartilage repair.In addition,the specific action mechanisms and design regimens of 2D-layered material-based nanoplatforms are clarified.Finally,the current challenges are discussed,and the key inspirations for further broadening the pre/clinical applications of 2D layered materials in orthopedic disorder therapy are proposed.
基金financial supports from the National Natural Science Foundation of China(31961133004,21977013,21903045)the National Key R&D Program of China(2018YFA0902200)+1 种基金China Post-doctoral Science Foundation(2019M661842)the Fundamental Research Funds for the Cornell University(PT1917,buctrc201,30920021122)。
文摘Engineering of enzyme microenvironment can surprisingly boost the apparent activity.However,the underlying regulation mechanism is not well-studied at a molecular level so far.Here,we present a modulation of two model enzymes of cytochrome c(Cty C)and D-amino acid oxidase(DAAO)with opposite pH-activity profiles using ionic polymers.The operational pH of poly(acrylic acid)modified Cyt C and polyallylamine modified DAAO was extended to 3-7 and 2-10 where the enzyme activity was larger than that at their optimum pH of 4.5 and 8.5 by 106%and 28%,respectively.The cascade reaction catalyzed by two modified enzymes reveals a 1.37-fold enhancement in catalytic efficiency compared with their native counterparts.The enzyme activity boosting is understood by performing the UV-vis/CD spectroscopy and molecular dynamics simulations in the atomistic level.The increased activity is ascribed to the favorable microenvironment in support of preserving enzyme native structures nearby cofactor under external perturbations.
