Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advanta...Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.展开更多
Among the various types of heterogeneous catalysts,supported metal nanocatalysts(SMNCs)have attracted widespread interest in chemistry and materials science,due to their advantageous features,such as high efficiency,s...Among the various types of heterogeneous catalysts,supported metal nanocatalysts(SMNCs)have attracted widespread interest in chemistry and materials science,due to their advantageous features,such as high efficiency,stability,and reusability for catalytic reactions.However,to obtain well-defined SMNCs and inhibit nanoparticle aggregation,traditional approaches generally involve numerous organic reagents,complex steps,and specialized equipment,thus hindering the practical and large-scale synthesis of SMNCs.In this review,we summarize green and sustainable synthetic methodologies for the assembly of SMNCs,including low temperature pyrolysis and solid-state,surfactant-and reductant-free,and ionic liquid assisted syntheses.The conventional application of SMNCs for electrochemical hydrogen evolution and the corresponding achievements are subsequently discussed.Finally,future perspectives toward the sustainable production of SMNCs are presented.展开更多
Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2w...Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2were composed of irregular nanosheets.The Bi4O5Br2nanosheets exhibited high and stable visible‐light photocatalytic efficiency for ppb‐level NO removal.The performance of Bi4O5Br2was markedly higher than that of the Bi12O17Br2nanosheets.The hydroxyl radical(?OH)was determined to be the main reactive oxygen species for the photo‐degradation processes of both Bi12O17Br2and Bi4O5Br2.However,in situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that Bi12O17Br2and Bi4O5Br2featured different conversion pathways for visible light driven photocatalytic NO oxidation.The excellent photocatalytic activity of Bi4O5Br2resulted from a high surface area and large pore volumes,which facilitated the transport of reactants and intermediate products,and provided more active sites for photochemical reaction.Furthermore,the Bi4O5Br2nanosheets produced more?OH and presented stronger valence band holeoxidation.In addition,the oxygen atoms of NO could insert into oxygen‐vacancies of Bi4O5Br2,whichprovided more active sites for the reaction.This work gives insight into the photocatalytic pollutant‐degradation mechanism of bismuth oxyhalide.展开更多
Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting el...Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.展开更多
The aspartic acid(ASP),an environment-friendly corrosion inhibitor,was explored to intercalate into the ZnAl-layered double hydroxide(ZnAl-LDH)and MgAl-LDH coatings on AZ31 magnesium alloys by a facile one-step hydrot...The aspartic acid(ASP),an environment-friendly corrosion inhibitor,was explored to intercalate into the ZnAl-layered double hydroxide(ZnAl-LDH)and MgAl-LDH coatings on AZ31 magnesium alloys by a facile one-step hydrothermal method.The morphology,composition,structure and corrosion resistance of the prepared coatings were comparatively investigated.It is found that the uniform and dense layered nanosheet(NS)vertically grows on the substrate,and the MgAl−ASP-LDH films exhibit a three-dimensional(3D)rose-like sheet structure with high ratio of pore coverage.The MgAl−ASP-LDH coating exhibits better corrosion resistance and durability of longtime immersion than ZnAl−ASP-LDH coating.The corrosion current density of two coatings is two or three orders of magnitude lower than that of bare Mg alloy,indicating that ZnAl/MgAl-LDH films intercalated with organic ASP anions can significantly improve the corrosion resistance of Mg alloy.展开更多
To realize the high-efficiency photodegradation of antibiotics,a novel S-scheme heterojunction photocatalyst g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) was proposed and successfully prepared in this work.The 10%g-C_(3)N_(4)/B...To realize the high-efficiency photodegradation of antibiotics,a novel S-scheme heterojunction photocatalyst g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) was proposed and successfully prepared in this work.The 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) heterojunction exhibits the highest degradation rate of norfloxacin(NOR)and bisphenol A(BPA).The degradation rate of NOR on 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) is about 1.38 and 2.33 times higher than that of pure Bi_(8)(CrO_(4))O_(11) and g-C_(3)N_(4),respectively.Further,the degradation rate of BPA over 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) heterojunction is bout 1.35 and 9.11 times higher than that of pure Bi_(8)(CrO_(4))O_(11) and g-C_(3)N_(4),respectively.The formation of S-scheme heterojunction facilitates the separation of photogenerated electron-hole pairs and reduces the recombination of charge carriers,which was confirmed by photocurrent,electrochemical impedance spectroscopy,steady-state and time-resolved transient photoluminescence spectrum,etc.The in-situ X-ray photoelectron spectroscopy,radical trapping experiments and electron paramagnetic resonance results demonstrate that the charge transfer is in accord with S-scheme mechanism.展开更多
The original description of male hypopygium of Tipula(Emodotipula) holoteles Alexander, 1924 is expanded with additional morphological characters and detailed illustrations. The additional morphological descriptions o...The original description of male hypopygium of Tipula(Emodotipula) holoteles Alexander, 1924 is expanded with additional morphological characters and detailed illustrations. The additional morphological descriptions of the female ovipositor along with detailed drawings are provided. The male semen pump and the female vaginal apodeme as well as the spermatheca are also described and illustrated for the first time, representing the first report of these structures of Tipula(Emodotipula) holoteles. Additionally, the taxonomic potential of the semen pump in the subgenus Emodotipula is analyzed and discussed. The new specific name Tipula(Emodotipula) yangi nom. nov. is proposed as a replacement name for junior homonym Tipula(Emodotipula) alexanderi Men, 2017. A worldwide checklist and a key to Chinese species of the subgenus Emodotipula are provided.展开更多
Two new species in the subgenus Formotipula Matsumura,1916,T.(Formotipula)gongshanensis sp.nov.from Yunnan and T.(F.)medogensis sp.nov.from Tibet,are described and illustrated.Males of T.(F.)spoliatrix Alexander,1941 ...Two new species in the subgenus Formotipula Matsumura,1916,T.(Formotipula)gongshanensis sp.nov.from Yunnan and T.(F.)medogensis sp.nov.from Tibet,are described and illustrated.Males of T.(F.)spoliatrix Alexander,1941 and T.(F.)stoneana Alexander,1943 are redescribed and illustrated based on additional morphological characters.Females of T.(F.)stoneana and T.(F.)decurvans Alexander,1950 are reported for the first time.展开更多
A new species of the genus Tipulodina Enderlein, 1912, Tipulodina simianshanensis Men sp. nov.(South China: Chongqing) is described and illustrated. A key to known species of the genus in China is provided. The new sp...A new species of the genus Tipulodina Enderlein, 1912, Tipulodina simianshanensis Men sp. nov.(South China: Chongqing) is described and illustrated. A key to known species of the genus in China is provided. The new species represents the first record of Tipulodina species from Chongqing, China.展开更多
The large genus Tipula Linnaeus,1758 contributes heavily to the biodiversity of the family Tipulidae.However,the monophyly of Tipula has not yet been verified.The subgenus Sivatipula Alexander,1964 is possibly the mos...The large genus Tipula Linnaeus,1758 contributes heavily to the biodiversity of the family Tipulidae.However,the monophyly of Tipula has not yet been verified.The subgenus Sivatipula Alexander,1964 is possibly the most confusing subgeneric taxon in the genus Tipula because of its members’particularly long antenna and one-armed posterior immovable apodeme on semen pump,which makes its subgeneric position uncertain.In this research,the sequences of cytochrome oxidase I(COI)for 19 Tipula species and five taxa from other genera are analyzed.Considering the molecular evidence on genetic distance as well as phylogenetic analysis and morphological information,our results indicate that(1)the genus Tipula is not resolved as monophyletic in phylogeny based on neighbor joining(NJ)and maximum likelihood(ML)trees because the subgenus Sivatipula doesn’t form a monophyletic clade with the remaining subgenera of Tipula;and(2)Sivatipula may deserve a generic status since it forms an independent phylogenetic line.展开更多
A new species in the genus Tipulodina Enderlein,1912,Tipulodina bispina sp.nov.(Guangxi,South China),is described and illustrated.The description,illustrations and drawings for this new species are provided.It is dist...A new species in the genus Tipulodina Enderlein,1912,Tipulodina bispina sp.nov.(Guangxi,South China),is described and illustrated.The description,illustrations and drawings for this new species are provided.It is distinguished from related species by the shapes of the gonostylus.展开更多
基金supported by the National Natural Science Foundation of China(21501016,21777011 and 21822601)the National Key R&D Program of China(2016YFC02047)+2 种基金the Innovative Research Team of Chongqing(CXTDG201602014)the Key Natural Science Foundation of Chongqing(cstc2017jcyj BX0052)the National Ten Thousand Talent Program of China~~
文摘Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.
文摘Among the various types of heterogeneous catalysts,supported metal nanocatalysts(SMNCs)have attracted widespread interest in chemistry and materials science,due to their advantageous features,such as high efficiency,stability,and reusability for catalytic reactions.However,to obtain well-defined SMNCs and inhibit nanoparticle aggregation,traditional approaches generally involve numerous organic reagents,complex steps,and specialized equipment,thus hindering the practical and large-scale synthesis of SMNCs.In this review,we summarize green and sustainable synthetic methodologies for the assembly of SMNCs,including low temperature pyrolysis and solid-state,surfactant-and reductant-free,and ionic liquid assisted syntheses.The conventional application of SMNCs for electrochemical hydrogen evolution and the corresponding achievements are subsequently discussed.Finally,future perspectives toward the sustainable production of SMNCs are presented.
基金supported by the National Natural Science Foundation of China(51708078,21576034)Chongqing Postdoctoral Science Foundation funded project(Xm2016027)the Innovative Research Team of Chongqing(CXTDG201602014,CXTDX201601016)~~
文摘Bi12O17Br2and Bi4O5Br2visible‐light driven photocatalysts,were respectively fabricated by hydrothermal and room‐temperature deposition methods with the use of BiBr3and NaOH as precursors.Both Bi12O17Br2and Bi4O5Br2were composed of irregular nanosheets.The Bi4O5Br2nanosheets exhibited high and stable visible‐light photocatalytic efficiency for ppb‐level NO removal.The performance of Bi4O5Br2was markedly higher than that of the Bi12O17Br2nanosheets.The hydroxyl radical(?OH)was determined to be the main reactive oxygen species for the photo‐degradation processes of both Bi12O17Br2and Bi4O5Br2.However,in situ diffuse reflectance infrared Fourier transform spectroscopy analysis revealed that Bi12O17Br2and Bi4O5Br2featured different conversion pathways for visible light driven photocatalytic NO oxidation.The excellent photocatalytic activity of Bi4O5Br2resulted from a high surface area and large pore volumes,which facilitated the transport of reactants and intermediate products,and provided more active sites for photochemical reaction.Furthermore,the Bi4O5Br2nanosheets produced more?OH and presented stronger valence band holeoxidation.In addition,the oxygen atoms of NO could insert into oxygen‐vacancies of Bi4O5Br2,whichprovided more active sites for the reaction.This work gives insight into the photocatalytic pollutant‐degradation mechanism of bismuth oxyhalide.
文摘Efficient,stable,and noble‐metal‐free electrocatalysts for both the oxygen evolution reaction and the hydrogen evolution reaction are highly imperative for the realization of low‐cost commercial water‐splitting electrolyzers.Herein,a cost‐effective and ecofriendly strategy is reported to fabricate coral‐like FeNi(OH)x/Ni as a bifunctional electrocatalyst for overall water splitting in alkaline media.With the assistance of mild corrosion of Ni by Fe(NO3)3,in situ generated FeNi(OH)x nanosheets are intimately attached on metallic coral‐like Ni.Integration of these nanosheets with the electrodeposited coral‐like Ni skeleton and the supermacroporous Ni foam substrate forms a binder‐free hierarchical electrode,which is beneficial for exposing catalytic active sites,accelerating mass transport,and facilitating the release of gaseous species.In 1.0 mol L^-1 KOH solution,a symmetric electrolyzer constructed with FeNi(OH)x/Ni as both the anode and the cathode exhibits an excellent activity with an applied potential difference of 1.52 V at 10 mA cm^-2,which is superior to that of an asymmetric electrolyzer constructed with the state‐of‐the‐art RuO2‐PtC couple(applied potential difference of 1.55 V at 10 mA cm^-2).This work contributes a facile and reliable strategy for manufacturing affordable,practical,and promising water‐splitting devices.
基金Projects(cstc2019jcyj-msxmX0566,cstc2018jcyjAX0450,cstc2018jcyjA2923,cstc2017jcyjAX0393)supported by the Natural Science Foundation of Chongqing City,ChinaProject(2019CDXZWL002)supported by President Foundation of Chongqing University,China+2 种基金Projects(2019CDXYWL0029,2018CDJDWL0011)supported by Fundamental Research Funds for the Central Universities of ChinaProjects(KJKJQN201800102,KJQN201800619,KJ1703042)supported by Science and Technology Research Program of Chongqing Municipal Education Commission,ChinaProjects(202003150060,202003150078)supported by Sharing Fund of Large-scale Equipment of Chongqing University,China。
文摘The aspartic acid(ASP),an environment-friendly corrosion inhibitor,was explored to intercalate into the ZnAl-layered double hydroxide(ZnAl-LDH)and MgAl-LDH coatings on AZ31 magnesium alloys by a facile one-step hydrothermal method.The morphology,composition,structure and corrosion resistance of the prepared coatings were comparatively investigated.It is found that the uniform and dense layered nanosheet(NS)vertically grows on the substrate,and the MgAl−ASP-LDH films exhibit a three-dimensional(3D)rose-like sheet structure with high ratio of pore coverage.The MgAl−ASP-LDH coating exhibits better corrosion resistance and durability of longtime immersion than ZnAl−ASP-LDH coating.The corrosion current density of two coatings is two or three orders of magnitude lower than that of bare Mg alloy,indicating that ZnAl/MgAl-LDH films intercalated with organic ASP anions can significantly improve the corrosion resistance of Mg alloy.
文摘To realize the high-efficiency photodegradation of antibiotics,a novel S-scheme heterojunction photocatalyst g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) was proposed and successfully prepared in this work.The 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) heterojunction exhibits the highest degradation rate of norfloxacin(NOR)and bisphenol A(BPA).The degradation rate of NOR on 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) is about 1.38 and 2.33 times higher than that of pure Bi_(8)(CrO_(4))O_(11) and g-C_(3)N_(4),respectively.Further,the degradation rate of BPA over 10%g-C_(3)N_(4)/Bi_(8)(CrO_(4))O_(11) heterojunction is bout 1.35 and 9.11 times higher than that of pure Bi_(8)(CrO_(4))O_(11) and g-C_(3)N_(4),respectively.The formation of S-scheme heterojunction facilitates the separation of photogenerated electron-hole pairs and reduces the recombination of charge carriers,which was confirmed by photocurrent,electrochemical impedance spectroscopy,steady-state and time-resolved transient photoluminescence spectrum,etc.The in-situ X-ray photoelectron spectroscopy,radical trapping experiments and electron paramagnetic resonance results demonstrate that the charge transfer is in accord with S-scheme mechanism.
基金supported by the National Natural Science Foundation of China (31300551)the Anhui Outstanding Young Talent Support Program (gxfx2017059)
文摘The original description of male hypopygium of Tipula(Emodotipula) holoteles Alexander, 1924 is expanded with additional morphological characters and detailed illustrations. The additional morphological descriptions of the female ovipositor along with detailed drawings are provided. The male semen pump and the female vaginal apodeme as well as the spermatheca are also described and illustrated for the first time, representing the first report of these structures of Tipula(Emodotipula) holoteles. Additionally, the taxonomic potential of the semen pump in the subgenus Emodotipula is analyzed and discussed. The new specific name Tipula(Emodotipula) yangi nom. nov. is proposed as a replacement name for junior homonym Tipula(Emodotipula) alexanderi Men, 2017. A worldwide checklist and a key to Chinese species of the subgenus Emodotipula are provided.
基金This study is supported by grants from the National Natural Science Foundation of China(31300551)the Anhui Outstanding Young Talent Support Program(gxfx2017059).
文摘Two new species in the subgenus Formotipula Matsumura,1916,T.(Formotipula)gongshanensis sp.nov.from Yunnan and T.(F.)medogensis sp.nov.from Tibet,are described and illustrated.Males of T.(F.)spoliatrix Alexander,1941 and T.(F.)stoneana Alexander,1943 are redescribed and illustrated based on additional morphological characters.Females of T.(F.)stoneana and T.(F.)decurvans Alexander,1950 are reported for the first time.
基金supported by the National Natural Science Foundation of China(31300551)the Anhui Outstanding Young Talent Support Program(gxfx2017059)
文摘A new species of the genus Tipulodina Enderlein, 1912, Tipulodina simianshanensis Men sp. nov.(South China: Chongqing) is described and illustrated. A key to known species of the genus in China is provided. The new species represents the first record of Tipulodina species from Chongqing, China.
基金supported by the National Natural Science Foundation of China(31300551)the Anhui Outstanding Young Talent Support Program(gxbjZD2020073)。
文摘The large genus Tipula Linnaeus,1758 contributes heavily to the biodiversity of the family Tipulidae.However,the monophyly of Tipula has not yet been verified.The subgenus Sivatipula Alexander,1964 is possibly the most confusing subgeneric taxon in the genus Tipula because of its members’particularly long antenna and one-armed posterior immovable apodeme on semen pump,which makes its subgeneric position uncertain.In this research,the sequences of cytochrome oxidase I(COI)for 19 Tipula species and five taxa from other genera are analyzed.Considering the molecular evidence on genetic distance as well as phylogenetic analysis and morphological information,our results indicate that(1)the genus Tipula is not resolved as monophyletic in phylogeny based on neighbor joining(NJ)and maximum likelihood(ML)trees because the subgenus Sivatipula doesn’t form a monophyletic clade with the remaining subgenera of Tipula;and(2)Sivatipula may deserve a generic status since it forms an independent phylogenetic line.
基金supported by the National Natural Science Foundation of China(31300551)the Scientific Research Foundation of the Higher Education Institutions of Anhui Province(KJ2021A0646)the Anhui Outstanding Young Talent Support Program(gxbjZD2020073)。
文摘A new species in the genus Tipulodina Enderlein,1912,Tipulodina bispina sp.nov.(Guangxi,South China),is described and illustrated.The description,illustrations and drawings for this new species are provided.It is distinguished from related species by the shapes of the gonostylus.