Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and c...Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and corrosion.Here,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater electrolysis.Such a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl^(-),resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing test.Further,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V vs.RHE,a potential that is far beyond the thermodynamic potential of chlorine ion oxidatio n.This concept and approach to reasonably designing weaknucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the development of green hydrogen technique.展开更多
Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine chemicals.Herein,we focus on a...Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine chemicals.Herein,we focus on an electrochemical redox activation strategy to rationally manipulate the microstructure and surface valence states of copper foam(CF)and boost the corresponding performance towards electrocatalytic benzyl alcohol oxidation(EBA),accompanied by the efficient hydrogen production.Correspondingly,the Cu(II)‐dominated species are gradually formed on the CF surface with the dissolution and redeposition of copper in the suitable potential range.The new species containing Cu2O,CuO,and Cu(OH)2 during surface reconstruction process of the CF were confirmed by multiple characterization techniques.After 220‐cycled activation(CF‐220),the activated CF achieves an increase of current density for EBA in anode from 9.5 for the original CF to 29.3 mmol/cm2,while the pure hydrogen yield increases threefold than that of the original CF at 1.5 VRHE.The produced new species can endow the CF‐220 with abundant acidity sites,which can enhance the adsorption toward Lewis‐basicity benzyl alcohol,confirmed by NH3‐temperature‐programmed desorption.In situ Raman result further reveals that the as‐produced CuO,Cu(OH)2,and Cu(OH)42−are the main active species toward the EBA process.展开更多
The Hippo signaling pathway was discovered to control organ size in Drosophila through regulating cell proliferation and apoptosis (Yu et al., 2015). Arising studies over the past two decades have defined the core c...The Hippo signaling pathway was discovered to control organ size in Drosophila through regulating cell proliferation and apoptosis (Yu et al., 2015). Arising studies over the past two decades have defined the core components and regulation mechanisms of the pathway in both Drosophila and mammals.展开更多
The evolutionarily conserved Hippo signaling pathway plays an important role in organ size control by regulating cell proliferation and apoptosis.Here,we identify Lingerer(Lig)as a growth suppressor using RNAi modifyi...The evolutionarily conserved Hippo signaling pathway plays an important role in organ size control by regulating cell proliferation and apoptosis.Here,we identify Lingerer(Lig)as a growth suppressor using RNAi modifying screen in Drosophila melanogaster.Loss of lig increases organ size and upregulates bantam(ban)and the expression of the Hippo pathway target genes,while overexpression of lig results in diminished ban expression and organ size reduction.We demonstrate that Lig C-terminal exhibits dominant-negative function on growth and ban expression,and thus plays an important role in organ size control and ban regulation.In addition,we provide evidence that both Yki and Mad are essential for Lig-induced ban expression.We also show that Lig regulates the expression of the Hippo pathway target genes partially via Yorkie.Moreover,we find that Lig physically interacts with and requires Salvador to restrict cell growth.Taken together,we demonstrate that Lig functions as a critical growth suppressor to control organ size via ban and Hippo signaling.展开更多
The water promotion effects,where water can provide a solution-mediated reaction pathway in various heterogeneous chemical catalysis,have been presented and attracted wide attention recently,yet,the rational design of...The water promotion effects,where water can provide a solution-mediated reaction pathway in various heterogeneous chemical catalysis,have been presented and attracted wide attention recently,yet,the rational design of catalysts with a certain ability of enhancing water-induced reaction process is full of challenges and difficulties.Here,we show that by incorporating alkali(Na,K)cations as an electronic and/or structural promoter into Pd/rGO-ZnCr_(2)O_(4)(r GO,reduced graphene oxide),the obtained Pd(Na)/rGO-ZnCr_(2)O_(4)as a representative example demonstrates an outstanding benzyl alcohol oxidation activity in the Pickering emulsion system in comparison to the alkali-free counterpart.The response experiments of water injection confirm the enhanced activity,and the Na-modified catalyst can further enhance the promotion effects of water on the reaction.The effects of alkali cations for Pd nanoparticles are identified and deciphered by a series of experimental characterizations(XPS,in situ CO-DRIFTS,and CO-TPR coupled with MS),showing that there is abundant-OH on the surface of the catalyst,which is stabilized by the formation of Pd-OH_(x).The alkali-stabilized Pd-OH_(x)is helpful to enhance the waterinduced reaction process.According to the results of in situ Raman as well as UV-vis absorption spectra,the Na-modulated Pd(Na)/rGO-ZnCr_(2)O_(4)enables the beneficial characteristics for distorting the benzyl alcohol structure and enhancing the adsorption of benzyl alcohol.Further,the mechanism for enhanced water promotion effects is rationally proposed.The strategy of alkali cations-modified catalysts can provide a new direction to effectively enhance the chemical reaction involving small molecule water.展开更多
基金supported by the National Natural Science Foundation of China(NSFC,No.22078052)the Fundamental Research Funds for the Central Universities(DUT22ZD207,DUT22LAB612)。
文摘Seawater splitting into hydrogen,a promising technology,is seriously limited by the durability and tolerance of electrocatalysts for chlorine ions in seawater at large current densities due to chloride oxidation and corrosion.Here,we present a robust and weak-nucleophilicity nickel-iron hydroxide electrocatalyst with excellent selectivity for oxygen evolution and an inert response for chlorine ion oxidation which are key and highly desired for efficient seawater electrolysis.Such a weak-nucleophilicity electrocatalyst can well match with strong-nucleophilicity OH-compared with the weak-nucleophilicity Cl^(-),resultantly,the oxidation of OH-in electrolyte can be more easily achieved relative to chlorine ion oxidation,confirmed by ethylenediaminetetraacetic acid disodium probing test.Further,no strongly corrosive hypochlorite is produced when the operating voltage reaches about 2.1 V vs.RHE,a potential that is far beyond the thermodynamic potential of chlorine ion oxidatio n.This concept and approach to reasonably designing weaknucleophilicity electrocatalysts that can greatly avoid chlorine ion oxidation under alkaline seawater environments can push forward the seawater electrolysis technology and also accelerate the development of green hydrogen technique.
基金supported by the National Natural Science Foundation of China(Nos.22078052,U2003216)the Fundamental Research Funds for the Central Universities(No.DUT22ZD207)Shandong Provincial Natural Science Foundation(No.ZR2020ZD08).
文摘Electrocatalytic water splitting that is coupled with electrocatalytic chemical oxidation is considered as one of the promising methods for efficiently obtaining hydrogen energy and fine chemicals.Herein,we focus on an electrochemical redox activation strategy to rationally manipulate the microstructure and surface valence states of copper foam(CF)and boost the corresponding performance towards electrocatalytic benzyl alcohol oxidation(EBA),accompanied by the efficient hydrogen production.Correspondingly,the Cu(II)‐dominated species are gradually formed on the CF surface with the dissolution and redeposition of copper in the suitable potential range.The new species containing Cu2O,CuO,and Cu(OH)2 during surface reconstruction process of the CF were confirmed by multiple characterization techniques.After 220‐cycled activation(CF‐220),the activated CF achieves an increase of current density for EBA in anode from 9.5 for the original CF to 29.3 mmol/cm2,while the pure hydrogen yield increases threefold than that of the original CF at 1.5 VRHE.The produced new species can endow the CF‐220 with abundant acidity sites,which can enhance the adsorption toward Lewis‐basicity benzyl alcohol,confirmed by NH3‐temperature‐programmed desorption.In situ Raman result further reveals that the as‐produced CuO,Cu(OH)2,and Cu(OH)42−are the main active species toward the EBA process.
基金This work was supported by the 'Strategic Priority Research Program' of the Chinese Academy of Sciences (XDB19000000), the National Key Research and Development Program of China (2017YFA0103601), the National Natural Science Foundation of China (31530043 and 31625017), the 'Cross and Cooperation in Science and Technology Innovation Team' Project of the Chinese Academy of Sciences, and the CAS/SAFEA International Partnership Program for Creative Research Teams.
文摘The Hippo signaling pathway was discovered to control organ size in Drosophila through regulating cell proliferation and apoptosis (Yu et al., 2015). Arising studies over the past two decades have defined the core components and regulation mechanisms of the pathway in both Drosophila and mammals.
基金This work is supported by grants from the National Basic Research Program of China(973 Program)(2010CB912101,2012CB945001,2011CB943902)the‘Strategic Priority Research Program’of the Chinese Academy of Sciences(XDA01010406)National Natural Science Foundation of China(31171394,31371462).
文摘The evolutionarily conserved Hippo signaling pathway plays an important role in organ size control by regulating cell proliferation and apoptosis.Here,we identify Lingerer(Lig)as a growth suppressor using RNAi modifying screen in Drosophila melanogaster.Loss of lig increases organ size and upregulates bantam(ban)and the expression of the Hippo pathway target genes,while overexpression of lig results in diminished ban expression and organ size reduction.We demonstrate that Lig C-terminal exhibits dominant-negative function on growth and ban expression,and thus plays an important role in organ size control and ban regulation.In addition,we provide evidence that both Yki and Mad are essential for Lig-induced ban expression.We also show that Lig regulates the expression of the Hippo pathway target genes partially via Yorkie.Moreover,we find that Lig physically interacts with and requires Salvador to restrict cell growth.Taken together,we demonstrate that Lig functions as a critical growth suppressor to control organ size via ban and Hippo signaling.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.51872035 and 22078052)the Innovation Program of Dalian City of Liaoning Province(No.2019RJ03)。
文摘The water promotion effects,where water can provide a solution-mediated reaction pathway in various heterogeneous chemical catalysis,have been presented and attracted wide attention recently,yet,the rational design of catalysts with a certain ability of enhancing water-induced reaction process is full of challenges and difficulties.Here,we show that by incorporating alkali(Na,K)cations as an electronic and/or structural promoter into Pd/rGO-ZnCr_(2)O_(4)(r GO,reduced graphene oxide),the obtained Pd(Na)/rGO-ZnCr_(2)O_(4)as a representative example demonstrates an outstanding benzyl alcohol oxidation activity in the Pickering emulsion system in comparison to the alkali-free counterpart.The response experiments of water injection confirm the enhanced activity,and the Na-modified catalyst can further enhance the promotion effects of water on the reaction.The effects of alkali cations for Pd nanoparticles are identified and deciphered by a series of experimental characterizations(XPS,in situ CO-DRIFTS,and CO-TPR coupled with MS),showing that there is abundant-OH on the surface of the catalyst,which is stabilized by the formation of Pd-OH_(x).The alkali-stabilized Pd-OH_(x)is helpful to enhance the waterinduced reaction process.According to the results of in situ Raman as well as UV-vis absorption spectra,the Na-modulated Pd(Na)/rGO-ZnCr_(2)O_(4)enables the beneficial characteristics for distorting the benzyl alcohol structure and enhancing the adsorption of benzyl alcohol.Further,the mechanism for enhanced water promotion effects is rationally proposed.The strategy of alkali cations-modified catalysts can provide a new direction to effectively enhance the chemical reaction involving small molecule water.