The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts c...The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.展开更多
This paper lays particular emphasis on pun's effectiveness and selectivity in English advertisements.The illustration and examples can help us understand the English advertisements well and foster our ability to a...This paper lays particular emphasis on pun's effectiveness and selectivity in English advertisements.The illustration and examples can help us understand the English advertisements well and foster our ability to appreciate the charm of English.展开更多
The green miridbug,Cyrtorhinus lividipennis,is an important predator of the rice brown planthopper,Nilaparvata lugens.In this study,the selective toxicity of seven commercial biopesticides for C.lividipennis was exami...The green miridbug,Cyrtorhinus lividipennis,is an important predator of the rice brown planthopper,Nilaparvata lugens.In this study,the selective toxicity of seven commercial biopesticides for C.lividipennis was examined under laboratory conditions; abamectin was the most selective to C.lividipennis,followed by matrine and azadirachtin.Veratridine,rotenone,Bacillus thuringiensis and Beauveria bassiana showed less selectivity for C.lividipennis.Subsequently,matrine,abamectin and azadirachtin were selected for sublethal assessments with respect to C.lividipennis due to their high toxicities to N.lugens.C.lividipennis treated with sublethal concentrations(LC10 and LC20) of the three biopesticides could distinguish volatiles released from healthy and N.lugens-infested plants indicating that the biopesticides tested did not affect the foraging ability of surviving miridbugs.Azadirachtin decreased the consumption capability of C.lividipennis when the densities of N.lugens were 20,30,40 and 50 insects per vial.Sublethal concentration treatment did not impact the pre-oviposition period or egg hatchability of C.lividipennis.However,the fecundity of C.lividipennis exposed to azadirachtin and abamectin increased by 27–41% compared to the untreated individuals.In summary,abamectin or matrine together with C.lividipennis could be considered an effective,sustainable pest management strategy for rice.展开更多
The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficien...The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.展开更多
Selective catalytic transfer hydrogenation(CTH)of carbonyl compounds to obtain specific alcohols holds significant importance across various fields.Achieving multiple selectivity in CTH is particularly crucial,but ful...Selective catalytic transfer hydrogenation(CTH)of carbonyl compounds to obtain specific alcohols holds significant importance across various fields.Achieving multiple selectivity in CTH is particularly crucial,but full of great challenge.Herein,a cationic In-captured Zr-porphyrin framework(1)with nanosized pores/cages was successfully constructed and showed high structure stability.Catalytic investigations revealed that 1 displayed highly multi-selective CTH of aldehydes and ketones containing both chemo-and size selectivity for the first time.The CTH of aldehydes and ketones exhibited remarkable reductive selectivity of 99%towards C=O bonds into CH–OH in the presence of-NO_(2),-CN and C=C groups.Through tuning the reaction conditions,1 also exhibited highly selective reduction of 97%for-CHO groups in the simultaneous presence of-CHO and-COCH3groups in intra-and intermolecular settings.Remarkably,reductive selectivity towards-CHO group remained prominent among five concurrent unsaturated groups mentioned above.Additionally,the definite pore size of 1 facilitated volume control of substrates,enabling size selectivity.1 as a heterogeneous catalyst was further confirmed by leaching tests,and maintained high activity even after being used for at least six cycles.Mechanistic studies have revealed that Zr6O8clusters served as the catalytic centers and the observed chemoselectivity mainly results from the synergistic effect of distinct metal sites within 1.The heightened selectivity towards-CHO over-COCH_(3)can be attributed to the easier realization of transfer hydrogenation processes for-CHO compared to-COCH_(3).展开更多
The flotation separation of cassiterite and dravite was realized using lead complexes of benzohydroxamic acid(Pb-BHA)as a collector and sodium fluosilicate(SF)as a depressant.Zeta potential tests confirmed that SF ena...The flotation separation of cassiterite and dravite was realized using lead complexes of benzohydroxamic acid(Pb-BHA)as a collector and sodium fluosilicate(SF)as a depressant.Zeta potential tests confirmed that SF enabled the selective depression of dravite.The results of Fourier transform infrared(FTIR)spectroscopy analysis demonstrated that hydroxyl-containing groups in the hydrolysis products of SF selectively chemisorbed on the surface of dravite.X-ray photoelectron spectroscopy(XPS)analysis results further demonstrated the strong chemisorption of SF hydrolysis products(F-containing groups and hydroxyl-containing groups)on dravite(Mg sites).Consequently,the adsorption of Pb-BHA on dravite was selectively prevented.Based on the results,a selective depression model of SF on cassiterite and dravite was proposed.展开更多
Understanding the synergistic effect between ligands at the atomic level to control the catalytic selectivity of catalysts remains a significant challenge due to the complexity of ligand interactions and limitations i...Understanding the synergistic effect between ligands at the atomic level to control the catalytic selectivity of catalysts remains a significant challenge due to the complexity of ligand interactions and limitations in current analytical techniques.Herein,using precisely structured metal nanoclusters as models,we discovered that altering the electronegativity of substituents on donor thiolate ligands can modulate the bond dissociation energy of coordinated phosphine ligands on the clusters.This change leads to the selective dissociation of ligands during the catalytic process,thereby enabling control over catalytic selectivity with an abrupt increase in formate production from~0%to 23%.This work provides crucial insights into understanding ligand interactions on metal nanoparticle surfaces at the atomic level and lays the foundation for designing highly selective catalysts in the future.展开更多
The tensile behavior of(Fe_(50)Mn_(30)Co_(10)Cr_(10))_(100-x)Si_(x)(x=0(Si0),2(Si2))metastable HEAs prepared by selective laser melting was studied at cryogenic temperatures.The results demonstrate that the addition o...The tensile behavior of(Fe_(50)Mn_(30)Co_(10)Cr_(10))_(100-x)Si_(x)(x=0(Si0),2(Si2))metastable HEAs prepared by selective laser melting was studied at cryogenic temperatures.The results demonstrate that the addition of Si leads to lattice distortion and a decrease in stacking fault energy,especially at 77 K,which significantly promotes transformation-induced plasticity(TRIP)in Si2 HEAs.The yield strength,tensile strength,and ductility of Si2 HEAs are 505.2 MPa,1364.1 MPa,and 19%,which are 43%,53% and 58% higher than those of Si0 alloy,respectively.TRIP is the main deformation mode,in addition to dislocation slip,and plays a key role in strengthening.The reinforced and continuously sustained TRIP maintains a dynamic strain distribution during deformation.Ultrahigh strain hardening greatly enhances the strength and ductility.展开更多
Chirality is a fundamental geometric property that manifests across molecular and nanoscale systems,profoundly influencing physical,chemical,and biological processes.At the intersection of chiral chemistry and nanosci...Chirality is a fundamental geometric property that manifests across molecular and nanoscale systems,profoundly influencing physical,chemical,and biological processes.At the intersection of chiral chemistry and nanoscience,chiral nanomaterials have emerged as a transformative class of materials,exhibiting unique spin-dependent properties governed by the chiral-induced spin selectivity(CISS)effect.This quantum phenomenon,rooted in spin-orbit coupling and spin filtering mechanisms,enables precise modulation of electron spin polarization,unlocking new opportunities in catalysis,spintronics,and energy conversion.This review provides a comprehensive overview of the CISS effect in chiral nanomaterials,elucidating its underlying mechanisms—including spin-orbit interactions,spin filtering,and spin blockade—and surveying advanced techniques for characterizing both structural chirality and spin polarization.We further highlight emerging applications in electrocatalysis,photocatalysis,and spintronic device engineering.Despite significant progress,key challenges remain in unraveling the fundamental physics,achieving accurate spin characterization,and translating these phenomena into robust,scalable technologies.Continued interdisciplinary research into the rational design and functionalization of chiral nanomaterials is poised to drive breakthroughs in sustainable energy,next-generation catalysis,and quantum information technologies.展开更多
Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(...Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.展开更多
N-K2Ti4O9/UiO-66-NH2 composites synthesized by a facile solvothermal method have a core-shell structure with UiO-66-NH2 forming the shell around a N-K2Ti4O9 core.Their photocatalytic activities in the degradation of d...N-K2Ti4O9/UiO-66-NH2 composites synthesized by a facile solvothermal method have a core-shell structure with UiO-66-NH2 forming the shell around a N-K2Ti4O9 core.Their photocatalytic activities in the degradation of dyes under visible light irradiation were investigated.The N-K2Ti4O9/UiO-66-NH2 composites exhibited higher photocatalytic activity than the pure components.This synergistic effect was due to the high adsorption capacity of UiO-66-NH2 and that the two components together induced an enhanced separation efficiency of photogenerated electron-hole pairs.The mass ratio of N-K2Ti4O9 to ZrCl4 of 3：7 in the composite exhibited the highest photocatalytic activity.Due to the electrostatic attraction between the negatively charged backbone of UiO-66-NH2with the positively charged groups of cationic dyes,the composites were more photocatalytically active for cationic dyes than for anionic dyes.展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
文摘The highly selective catalytic hydrogenation of halogenated nitroaromatics was achieved by employing Pd‑based catalysts that were co‑modified with organic and inorganic ligands.It was demonstrated that the catalysts contained Pd species in mixed valence states,with high valence Pd at the metal‑support interface and zero valence Pd at the metal surface.While the strong coordination of triphenylphosphine(PPh3)to Pd0 on the Pd surface prevents the adsorption of halogenated nitroaromatics and thus dehalogenation,the coordination of sodium metavanadate(NaVO3)to high‑valence Pd sites at the interface helps to activate H2 in a heterolytic pathway for the selective hydrogenation of nitro‑groups.The excellent catalytic performance of the interfacial active sites enables the selective hydrogenation of a wide range of halogenated nitroaromatics.
文摘This paper lays particular emphasis on pun's effectiveness and selectivity in English advertisements.The illustration and examples can help us understand the English advertisements well and foster our ability to appreciate the charm of English.
基金financially supported by the Jiangsu Agricultural Scientific Self-innovation Fund,China (CX(15)1057)the Fund of Science and Technology of Jiangsu Province,China (BE2015342)the National Key Research and Development Program of China (2017YFD0200400 and 2016YFD0300706)
文摘The green miridbug,Cyrtorhinus lividipennis,is an important predator of the rice brown planthopper,Nilaparvata lugens.In this study,the selective toxicity of seven commercial biopesticides for C.lividipennis was examined under laboratory conditions; abamectin was the most selective to C.lividipennis,followed by matrine and azadirachtin.Veratridine,rotenone,Bacillus thuringiensis and Beauveria bassiana showed less selectivity for C.lividipennis.Subsequently,matrine,abamectin and azadirachtin were selected for sublethal assessments with respect to C.lividipennis due to their high toxicities to N.lugens.C.lividipennis treated with sublethal concentrations(LC10 and LC20) of the three biopesticides could distinguish volatiles released from healthy and N.lugens-infested plants indicating that the biopesticides tested did not affect the foraging ability of surviving miridbugs.Azadirachtin decreased the consumption capability of C.lividipennis when the densities of N.lugens were 20,30,40 and 50 insects per vial.Sublethal concentration treatment did not impact the pre-oviposition period or egg hatchability of C.lividipennis.However,the fecundity of C.lividipennis exposed to azadirachtin and abamectin increased by 27–41% compared to the untreated individuals.In summary,abamectin or matrine together with C.lividipennis could be considered an effective,sustainable pest management strategy for rice.
文摘The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.
基金supported by National Nature Science Foundation of China(Nos.92161202 and 22121005)China Postdoctoral Science Foundation(Nos.2023M741814 and 2023M741815)+2 种基金Postdoctoral Fellowship Program of CPSF(No.GZC20231170)Natural Science Foundation of Science&Technology Department of Sichuan Province(No.2023NSFSC110)Research and Innovation Team of China West Normal University(No.KCXTD2023-1)。
文摘Selective catalytic transfer hydrogenation(CTH)of carbonyl compounds to obtain specific alcohols holds significant importance across various fields.Achieving multiple selectivity in CTH is particularly crucial,but full of great challenge.Herein,a cationic In-captured Zr-porphyrin framework(1)with nanosized pores/cages was successfully constructed and showed high structure stability.Catalytic investigations revealed that 1 displayed highly multi-selective CTH of aldehydes and ketones containing both chemo-and size selectivity for the first time.The CTH of aldehydes and ketones exhibited remarkable reductive selectivity of 99%towards C=O bonds into CH–OH in the presence of-NO_(2),-CN and C=C groups.Through tuning the reaction conditions,1 also exhibited highly selective reduction of 97%for-CHO groups in the simultaneous presence of-CHO and-COCH3groups in intra-and intermolecular settings.Remarkably,reductive selectivity towards-CHO group remained prominent among five concurrent unsaturated groups mentioned above.Additionally,the definite pore size of 1 facilitated volume control of substrates,enabling size selectivity.1 as a heterogeneous catalyst was further confirmed by leaching tests,and maintained high activity even after being used for at least six cycles.Mechanistic studies have revealed that Zr6O8clusters served as the catalytic centers and the observed chemoselectivity mainly results from the synergistic effect of distinct metal sites within 1.The heightened selectivity towards-CHO over-COCH_(3)can be attributed to the easier realization of transfer hydrogenation processes for-CHO compared to-COCH_(3).
基金supported by the National Natural Science Foundation of China(No.52122406)the National Key Research Center and Development Program of the 14th Five-year Plan of China(Nos.2022YFC2905104,2022YFC2905105).
文摘The flotation separation of cassiterite and dravite was realized using lead complexes of benzohydroxamic acid(Pb-BHA)as a collector and sodium fluosilicate(SF)as a depressant.Zeta potential tests confirmed that SF enabled the selective depression of dravite.The results of Fourier transform infrared(FTIR)spectroscopy analysis demonstrated that hydroxyl-containing groups in the hydrolysis products of SF selectively chemisorbed on the surface of dravite.X-ray photoelectron spectroscopy(XPS)analysis results further demonstrated the strong chemisorption of SF hydrolysis products(F-containing groups and hydroxyl-containing groups)on dravite(Mg sites).Consequently,the adsorption of Pb-BHA on dravite was selectively prevented.Based on the results,a selective depression model of SF on cassiterite and dravite was proposed.
基金financially supported by the National Natural Science Foundation of China(Nos.22301155,22171156,21803001)Taishan Scholar Foundation of Shandong Province(China)+2 种基金the Natural Science Foundation of Shandong Province(No.ZR2023QB122)Shandong Province Excellent Youth Innovation TeamStartup Funds from Qingdao University of Science and Technology
文摘Understanding the synergistic effect between ligands at the atomic level to control the catalytic selectivity of catalysts remains a significant challenge due to the complexity of ligand interactions and limitations in current analytical techniques.Herein,using precisely structured metal nanoclusters as models,we discovered that altering the electronegativity of substituents on donor thiolate ligands can modulate the bond dissociation energy of coordinated phosphine ligands on the clusters.This change leads to the selective dissociation of ligands during the catalytic process,thereby enabling control over catalytic selectivity with an abrupt increase in formate production from~0%to 23%.This work provides crucial insights into understanding ligand interactions on metal nanoparticle surfaces at the atomic level and lays the foundation for designing highly selective catalysts in the future.
基金supported by Program for Innovative Research Team in Science and Technology in Fujian Province University,Chinathe Natural Science Foundation of Fujian Province,China(Nos.2023J011013,2020J01898)。
文摘The tensile behavior of(Fe_(50)Mn_(30)Co_(10)Cr_(10))_(100-x)Si_(x)(x=0(Si0),2(Si2))metastable HEAs prepared by selective laser melting was studied at cryogenic temperatures.The results demonstrate that the addition of Si leads to lattice distortion and a decrease in stacking fault energy,especially at 77 K,which significantly promotes transformation-induced plasticity(TRIP)in Si2 HEAs.The yield strength,tensile strength,and ductility of Si2 HEAs are 505.2 MPa,1364.1 MPa,and 19%,which are 43%,53% and 58% higher than those of Si0 alloy,respectively.TRIP is the main deformation mode,in addition to dislocation slip,and plays a key role in strengthening.The reinforced and continuously sustained TRIP maintains a dynamic strain distribution during deformation.Ultrahigh strain hardening greatly enhances the strength and ductility.
基金supported by the Shanghai Pilot Program for Basic Research-Shanghai Jiao Tong University(21TQ1400211)the National Key Research and Development Program of China(2023YFB4004900)the Natural Science Foundation of Chongqing,China(CSTB2024NSCQ-MSX1115)。
文摘Chirality is a fundamental geometric property that manifests across molecular and nanoscale systems,profoundly influencing physical,chemical,and biological processes.At the intersection of chiral chemistry and nanoscience,chiral nanomaterials have emerged as a transformative class of materials,exhibiting unique spin-dependent properties governed by the chiral-induced spin selectivity(CISS)effect.This quantum phenomenon,rooted in spin-orbit coupling and spin filtering mechanisms,enables precise modulation of electron spin polarization,unlocking new opportunities in catalysis,spintronics,and energy conversion.This review provides a comprehensive overview of the CISS effect in chiral nanomaterials,elucidating its underlying mechanisms—including spin-orbit interactions,spin filtering,and spin blockade—and surveying advanced techniques for characterizing both structural chirality and spin polarization.We further highlight emerging applications in electrocatalysis,photocatalysis,and spintronic device engineering.Despite significant progress,key challenges remain in unraveling the fundamental physics,achieving accurate spin characterization,and translating these phenomena into robust,scalable technologies.Continued interdisciplinary research into the rational design and functionalization of chiral nanomaterials is poised to drive breakthroughs in sustainable energy,next-generation catalysis,and quantum information technologies.
基金financially supported by National Natural Science Foundation of China(22466010)Guizhou Provincial Basic Research Program(Natural Science)ZK[2023]47 and key program ZD[2025]075+6 种基金Innovation and Entrepreneurship Project for overseas Talents in Guizhou Province[2022]02Specific Natural Science Foundation of Guizhou University(X202207)the national undergraduate innovation and entrepreneurship training program(gzugc2023006gzusc2024012)SRT project of Guizhou university(2023SRT0292023SRT024)supported by Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Electrocatalytic nitrate reduction reaction(NO3RR)represents a sustainable and environmentally benign route for ammonia(NH3)synthesis.However,NO3RR is still limited by the competition from hydrogen evolution reaction(HER)and the high energy barrier in the hydrogenation step of nitrogen-containing intermediates.Here,we report a selective etching strategy to construct Ru M nanoalloys(M=Fe,Co,Ni,Cu)uniformly dispersed on porous nitrogen-doped carbon substrates for efficient neutral NH3electrosynthesis.Density functional theory calculations confirm that the synergic effect between Ru and transition metal M modulates the electronic structure of the alloy,significantly lowering the energy barrier for the conversion of*NO_(2)to*HNO_(2).Experimentally,the optimized Ru Fe-NC catalyst achieves 100%Faraday efficiency with a high yield rate of 0.83 mg h^(-1)mg^(-1)catat a low potential of-0.1 V vs.RHE,outperforming most reported catalysts.In situ spectroscopic analyses further demonstrate that the Ru M-NC effectively promotes the hydrogenation of nitrogen intermediates while inhibiting the formation of hydrogen radicals,thereby reducing HER competition.The Ru FeNC assembled Zn-NO_(3)^(-)battery achieved a high open-circuit voltage and an outstanding power density and capacity,which drive selective NO_(3)^(-)conversion to NH3.This work provides a powerful synergistic design strategy for efficient NH3electrosynthesis and a general framework for the development of advanced multi-component catalysts for sustainable nitrogen conversion.
基金supported by the National Natural Science Foundation of China (51372062)the Anhui Provincial Natural Science Foundation(1508085MB28,1308085MB21)~~
文摘N-K2Ti4O9/UiO-66-NH2 composites synthesized by a facile solvothermal method have a core-shell structure with UiO-66-NH2 forming the shell around a N-K2Ti4O9 core.Their photocatalytic activities in the degradation of dyes under visible light irradiation were investigated.The N-K2Ti4O9/UiO-66-NH2 composites exhibited higher photocatalytic activity than the pure components.This synergistic effect was due to the high adsorption capacity of UiO-66-NH2 and that the two components together induced an enhanced separation efficiency of photogenerated electron-hole pairs.The mass ratio of N-K2Ti4O9 to ZrCl4 of 3：7 in the composite exhibited the highest photocatalytic activity.Due to the electrostatic attraction between the negatively charged backbone of UiO-66-NH2with the positively charged groups of cationic dyes,the composites were more photocatalytically active for cationic dyes than for anionic dyes.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
