A growing population necessitates the development of sustainable agriculture,which requires achieving atom economy in pesticide delivery,fertilization,and so on.To this end,we focus on single-atom materials(SAMs)to en...A growing population necessitates the development of sustainable agriculture,which requires achieving atom economy in pesticide delivery,fertilization,and so on.To this end,we focus on single-atom materials(SAMs)to enhance atom utilization within agricultural systems.In this study,we report a novel pesticide for plants,a single-atom copper(Cu_(1))formulation,by employing a precipitation-equilibrium-driven(K_(sp)-driven)method to anchor Cu_(1)onto a calcium carbonate(CaCO_(3))carrier.Thanks to its high atom dispersion and utilization efficiency,the Cu_(1)formulation(Cu_(1)/CaCO_(3))significantly enhances crop disease resistance while exhibiting minimal phytotoxicity in the tested species.Notably,this formulation leads to nearly 20-fold less copper residue in the soil after field application compared to traditional copper formulations.It inhibits microbial growth potentially by targeting key bacterial membrane components through interactions with phosphate groups(–PO42–)in membrane phospholipids and binding to sulfhydryl(–SH)residues in respiratory chain proteins.Cu_(1)/CaCO_(3)represents SAMs as a promising tool for designing green pesticides to manage crop diseases and a novel interdisciplinary approach to promoting sustainable agriculture.展开更多
The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))und...The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))under industrial-level current density is urgently needed and pivotal.Herein,we report the Cu_(2)O nanoparticles doped with interstitial carbon atoms(denoted as C-Cu_(2)O NPs)for the conversion of CO_(2) to C_(2+)products.The interstitial carbon promotes the C-Cu_(2)O NPs to possess abundant unsaturated Cu–O bonds,leading to a high-density Cu^(δ+)(0<δ<1)species.The obtained C-Cu_(2)O NPs exhibited significant Faradic efficiency(FE)of C_(2+) products approaching 76.9%and a partial current density reaching 615.2 mA·cm^(–2)under an industrial-level current density of 800 mA·cm^(–2).Furthermore,the efficient electrosynthesis of C_(2)H_(4) achieved an FE of 57.4%with a partial current density of 459.2 mA·cm^(–2).In situ electrochemical attenuated total reflection Fourier transform infrared spectroscopy and in situ Raman spectroscopy analyses revealed that C-Cu_(2)O NPs stabilized the intermediate*CO and facilitated C–C coupling,leading to increased selectivity towards C_(2+) products.展开更多
Photocatalytic carbon dioxide(CO_(2))to carbon monoxide(CO)offers a promising way for both alleviating the greenhouse effect and meeting the industrial demand.Herein,we constructed a Co single-atom catalyst with inten...Photocatalytic carbon dioxide(CO_(2))to carbon monoxide(CO)offers a promising way for both alleviating the greenhouse effect and meeting the industrial demand.Herein,we constructed a Co single-atom catalyst with intentional low-coordination environment design on porous ZnO(denoted as Co1/ZnO).Impressively,Co1/ZnO exhibited a remarkable activity with a CO yield rate of 22.25 mmol·g^(-1)·h^(-1) and a selectivity of 80.2%for CO_(2) photoreduction reactions under visible light.The incorporation of single Co atoms provided an additional photo-generated electron transfer channel,which suppressed the carrier recombination of photocatalysts.Moreover,the unsaturated Co active sites were capable to adsorb CO_(2) molecule spontaneously,thus facilitating the activation of CO_(2) molecule during CO_(2) reduction course.展开更多
The performance of catalyst depends on the intrinsic activity of active sites and the structural characteristics of the support.Here,we simultaneously integrate single nickel(Ni)sites and platinum-nickel(PtNi)alloy na...The performance of catalyst depends on the intrinsic activity of active sites and the structural characteristics of the support.Here,we simultaneously integrate single nickel(Ni)sites and platinum-nickel(PtNi)alloy nanoparticles(NPs)on a two-dimensional(2D)porous carbon nanosheet,demonstrating remarkable catalytic performance in the oxygen reduction reaction(ORR).The single Ni sites can activate the oxygen molecules into key oxygen-containing intermediate that is further efficiently transferred to the adjacent PtNi alloy NPs and rapidly reduced to H_(2)O,which establishes a relay catalysis between active sites.The porous structure on the carbon nanosheet support promotes the transfer of active intermediates between these active sites,which assists the relay catalysis by improving mass diffusion.Remarkably,the obtained catalyst demonstrates a half-wave potential of up to 0.942 V,a high mass activity of 0.54 A·mgPt^(−1),and negligible decay of activity after 30,000 cycles,which are all superior to the commercial Pt/C catalysts with comparable loading of Pt.The theoretical calculation results reveal that the obtained catalyst with defect structure of carbon support presents enhanced relay catalytic effect of PtNi alloy NPs and single Ni sites,ultimately realizing improved catalytic performance.This work provides valuable inspiration for developing low platinum loading catalyst,integrating single atoms and alloy with outstanding performance in fuel cell.展开更多
基金supported by the Ministry of Science and Technology of China(2021YFA1500404)the University of Science and Technology of China(USTC)Research Funds of the Double First-Class Initiative(YD2060006005)+3 种基金the Joint Funds of the National Natural Science Foundation of China(NSFC)(U23A2081,92261105,and 22221003)the NSFC Center for Single-Atom Catalysis(22388102)the Fundamental Research Funds for the Central Universities(WK2060000088)the Anhui Provincial Key Research and Development Project(2023z04020010).
文摘A growing population necessitates the development of sustainable agriculture,which requires achieving atom economy in pesticide delivery,fertilization,and so on.To this end,we focus on single-atom materials(SAMs)to enhance atom utilization within agricultural systems.In this study,we report a novel pesticide for plants,a single-atom copper(Cu_(1))formulation,by employing a precipitation-equilibrium-driven(K_(sp)-driven)method to anchor Cu_(1)onto a calcium carbonate(CaCO_(3))carrier.Thanks to its high atom dispersion and utilization efficiency,the Cu_(1)formulation(Cu_(1)/CaCO_(3))significantly enhances crop disease resistance while exhibiting minimal phytotoxicity in the tested species.Notably,this formulation leads to nearly 20-fold less copper residue in the soil after field application compared to traditional copper formulations.It inhibits microbial growth potentially by targeting key bacterial membrane components through interactions with phosphate groups(–PO42–)in membrane phospholipids and binding to sulfhydryl(–SH)residues in respiratory chain proteins.Cu_(1)/CaCO_(3)represents SAMs as a promising tool for designing green pesticides to manage crop diseases and a novel interdisciplinary approach to promoting sustainable agriculture.
基金supported by the National Key R&D Program of China(No.2018YFA0702001)the National Natural Science Foundation of China(Nos.22371268 and 22301287)+4 种基金Fundamental Research Funds for the Central Universities(No.WK2060000016)Anhui Provincial Natural Science Foundation(Nos.2208085J09 and 2208085QB33)Collaborative Innovation Program of Hefei Science Center,CAS(No.2022HSC-CIP020)Youth Innovation Promotion Association of the Chinese Academy of Science(No.2018494)USTC Tang Scholar.
文摘The electrochemical CO_(2) reduction reaction(CO_(2)RR)holds significant promise in advancing carbon neutrality.Developing catalysts for the electrochemical CO_(2)RR to multi-carbon(C_(2+))products(e.g.,C_(2)H_(4))under industrial-level current density is urgently needed and pivotal.Herein,we report the Cu_(2)O nanoparticles doped with interstitial carbon atoms(denoted as C-Cu_(2)O NPs)for the conversion of CO_(2) to C_(2+)products.The interstitial carbon promotes the C-Cu_(2)O NPs to possess abundant unsaturated Cu–O bonds,leading to a high-density Cu^(δ+)(0<δ<1)species.The obtained C-Cu_(2)O NPs exhibited significant Faradic efficiency(FE)of C_(2+) products approaching 76.9%and a partial current density reaching 615.2 mA·cm^(–2)under an industrial-level current density of 800 mA·cm^(–2).Furthermore,the efficient electrosynthesis of C_(2)H_(4) achieved an FE of 57.4%with a partial current density of 459.2 mA·cm^(–2).In situ electrochemical attenuated total reflection Fourier transform infrared spectroscopy and in situ Raman spectroscopy analyses revealed that C-Cu_(2)O NPs stabilized the intermediate*CO and facilitated C–C coupling,leading to increased selectivity towards C_(2+) products.
基金supported by the National Natural Science Foundation of China(Nos.1222508,U1932213)the Fundamental Research Funds for the Central Universities(No.WK2060000016)+1 种基金the USTC Research Funds of the Double First-Class Initiative(No.YD2310002005)the Youth Innovation Promotion Association CAS(No.2020454)。
文摘Photocatalytic carbon dioxide(CO_(2))to carbon monoxide(CO)offers a promising way for both alleviating the greenhouse effect and meeting the industrial demand.Herein,we constructed a Co single-atom catalyst with intentional low-coordination environment design on porous ZnO(denoted as Co1/ZnO).Impressively,Co1/ZnO exhibited a remarkable activity with a CO yield rate of 22.25 mmol·g^(-1)·h^(-1) and a selectivity of 80.2%for CO_(2) photoreduction reactions under visible light.The incorporation of single Co atoms provided an additional photo-generated electron transfer channel,which suppressed the carrier recombination of photocatalysts.Moreover,the unsaturated Co active sites were capable to adsorb CO_(2) molecule spontaneously,thus facilitating the activation of CO_(2) molecule during CO_(2) reduction course.
基金supported by the National Key Research and Development Program of China(No.2021YFA1501003)the National Natural Science Foundation of China(Nos.92261105 and 22221003)+4 种基金the Anhui Provincial Natural Science Foundation(Nos.2108085UD06 and 2208085UD04)the Anhui Provincial Key Research and Development Project(Nos.2023z04020010 and 2022a05020053)the Collaborative Innovation Program of Hefei Science Center,CAS(No.2021HSC-CIP002)the Joint Funds from Hefei National Synchrotron Radiation Laboratory(Nos.KY2060000180 and KY2060000195)the Yanchang foundation(No.KD2203220074).
文摘The performance of catalyst depends on the intrinsic activity of active sites and the structural characteristics of the support.Here,we simultaneously integrate single nickel(Ni)sites and platinum-nickel(PtNi)alloy nanoparticles(NPs)on a two-dimensional(2D)porous carbon nanosheet,demonstrating remarkable catalytic performance in the oxygen reduction reaction(ORR).The single Ni sites can activate the oxygen molecules into key oxygen-containing intermediate that is further efficiently transferred to the adjacent PtNi alloy NPs and rapidly reduced to H_(2)O,which establishes a relay catalysis between active sites.The porous structure on the carbon nanosheet support promotes the transfer of active intermediates between these active sites,which assists the relay catalysis by improving mass diffusion.Remarkably,the obtained catalyst demonstrates a half-wave potential of up to 0.942 V,a high mass activity of 0.54 A·mgPt^(−1),and negligible decay of activity after 30,000 cycles,which are all superior to the commercial Pt/C catalysts with comparable loading of Pt.The theoretical calculation results reveal that the obtained catalyst with defect structure of carbon support presents enhanced relay catalytic effect of PtNi alloy NPs and single Ni sites,ultimately realizing improved catalytic performance.This work provides valuable inspiration for developing low platinum loading catalyst,integrating single atoms and alloy with outstanding performance in fuel cell.
基金supported by the National Key R&D Program of China(2017YFA0700104 and 2018YFA0702001)the National Natural Science Foundation of China(21871238)+2 种基金the Fundamental Research Funds for the Central Universities(WK2060000016)Natural Science Foundation of Anhui Province(2208085J09)USTC Tang Scholar。
