Response surface methodology(RSM) was employed to optimize the control parameters of TiO_2/graphene with exposed {001} facets during synthesis, and its enhanced photocatalytic activities were evaluated in the photodeg...Response surface methodology(RSM) was employed to optimize the control parameters of TiO_2/graphene with exposed {001} facets during synthesis, and its enhanced photocatalytic activities were evaluated in the photodegradation of toluene. Experimental results were in good agreement with the predicted results obtained using RSM with a correlation coefficient(R^2) of 0.9345. When 22.06 mg of graphite oxide(GO) and 2.09 mL of hydrofluoric acid(HF) were added and a hydrothermal time of 28 h was used, a maximum efficiency in the degradation of toluene was achieved. X-ray diffraction(XRD), transmission electron microscopy(TEM), and scanning electron microscopy(SEM) were employed to characterize the obtained hybrid photocatalyst. The electron transferred between Ti and C retarded the combination of electron–hole pairs and hastened the transferring of electrons, which enhanced the photocatalytic activity.展开更多
Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heter...Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heterostructure photoanodes.As a hole blocking layer of BiVO4,titanium dioxide(TiO_(2)) has been considered unsuitable because of its relatively positive valence band edge and low electrical conductivity.Herein,a crystal facet engineering of TiO_(2) nanostructures is proposed to control band structures for the hole blocking layer of BiVO4 nanodots.We design two types of TiO_(2) nanostructures,which are nanorods(NRs)and nanoflowers(NFs)with different(001)and(110)crystal facets,respectively,and fabricate BiVO4/TiO_(2) heterostructure photoanodes.The BiVO4/TiO_(2) NFs showed 4.8 times higher photocurrent density than the BiVO4/TiO_(2) NRs.Transient decay time analysis and time-resolved photoluminescence reveal the enhancement is attributed to the reduced charge recombination,which is originated from the formation of type II band alignment between BiVO4 nanodots and TiO_(2) NFs.This work provides not only new insights into the interplay between crystal facets and band structures but also important steps for the design of highly efficient photoelectrodes.展开更多
A large diamond crystal up to 500 μm in diameter with a smooth （100） facet at its top has been synthesized on Mo substrate through microwave plasma chemical vapor deposition （MPCVD）. Its morphology and quality we...A large diamond crystal up to 500 μm in diameter with a smooth （100） facet at its top has been synthesized on Mo substrate through microwave plasma chemical vapor deposition （MPCVD）. Its morphology and quality were characterized by scanning electron microscopy （SEM）, and the growth mechanism was roughly illustrated from both macroscopic and microscopic viewpoints. It was found that morphological instabilities are a major factor resulting in synthesis of large diamond crystals, moreover, high microwave power density （MPD）, high CH4 concentrations, high pressure, high substrate surface temperature and the addition of a small amount of O2 were also necessary for the synthesis of large diamond crystals.展开更多
A novel method was developed to deposit a large crystal diamond with good facets up to 1000 μm on a tungsten substrate using a microwave plasma enhanced chemical vapor deposition （MPCVD）. This method consists of tw...A novel method was developed to deposit a large crystal diamond with good facets up to 1000 μm on a tungsten substrate using a microwave plasma enhanced chemical vapor deposition （MPCVD）. This method consists of two steps, namely single-crystal nucleation and growth. Prior to the fabrication of the well-faceted, large crystal diamond, an investigation was made into the nucleation and growth of the diamond which were affected by the O2 concentration and substrate temperature. Deposited diamond crystals were characterized by scanning electron microscopy and micro-Raman spectroscopy. The results showed that the conditions of single-crystal nucleation were appropriate when the ratio of H2/CH4/O2 was about 200/7.0/2.0, while the sub- strate temperature Ts of 1000℃ to 1050℃ was the appropriate range for single-crystal diamond growth. Under the optimum parameters, a well-faeeted large crystal diamond was obtained.展开更多
The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality...The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.展开更多
This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated (001) facets for toluene degradation. The performance of photocatalyst wa...This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated (001) facets for toluene degradation. The performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mecha-nism were established by a combination of various characterization methods, in situ diuse reectance infrared fourier transform spectroscopy, and density functional theory calculation. The surface modtication with ozone can signiticantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5c-Ti sites on (001) facets act as the adsorption sites for ozone. The formed Ti-O bonds reacted with H2O to generate a large amount of isolated Ti5c-OH which act as the adsorption sites for toluene, and thus signi- cantly increase the adsorption capacity for toluene. The outstanding photo- catalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH· radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.展开更多
在KDP晶体（001）晶面上进行了四种压头（即：维氏压头、玻氏压头、圆锥压头、球形压头）的纳米压痕仿真研究。仿真结果表明：完全加载时四种压头与KDP晶体接触位置存在不同程度应力集中。当载荷在0-8 m N范围内时,其与等效应力影响深...在KDP晶体（001）晶面上进行了四种压头（即：维氏压头、玻氏压头、圆锥压头、球形压头）的纳米压痕仿真研究。仿真结果表明：完全加载时四种压头与KDP晶体接触位置存在不同程度应力集中。当载荷在0-8 m N范围内时,其与等效应力影响深度呈近似线性递增关系。完全卸载时,残余应力分布深度为1.3-1.5μm。相同载荷条件下,各压头对应的塑性损伤层深度之间关系与等效应力影响深度之间关系一致。此外,通过纳米压痕实验验证了KDP晶体材料模型及相关参数的正确性。展开更多
基金supported by the National Natural Science Foundation of China (Nos. 21406164, 21466035 and 51203111)the National Basic Research Program of China ("973" Program, Nos. 2012CB720100 and 2014CB239300)
文摘Response surface methodology(RSM) was employed to optimize the control parameters of TiO_2/graphene with exposed {001} facets during synthesis, and its enhanced photocatalytic activities were evaluated in the photodegradation of toluene. Experimental results were in good agreement with the predicted results obtained using RSM with a correlation coefficient(R^2) of 0.9345. When 22.06 mg of graphite oxide(GO) and 2.09 mL of hydrofluoric acid(HF) were added and a hydrothermal time of 28 h was used, a maximum efficiency in the degradation of toluene was achieved. X-ray diffraction(XRD), transmission electron microscopy(TEM), and scanning electron microscopy(SEM) were employed to characterize the obtained hybrid photocatalyst. The electron transferred between Ti and C retarded the combination of electron–hole pairs and hastened the transferring of electrons, which enhanced the photocatalytic activity.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science and ICT(MSIT)(2021R1A2B5B03001851)the NRF Grant funded by the Korean government MSIT(2021M3H4A1A03057403).M.G.L.acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education(2021R1A6A3A03039988).J.W.Y.acknowledges the Basic Science Research Program through the NRF funded by the Ministry of Education(2021R1A6A3A13046700).
文摘Although bismuth vanadate(BiVO4)has been promising as photoanode material for photoelectrochemical water splitting,its charge recombination issue by short charge diffusion length has led to various studies about heterostructure photoanodes.As a hole blocking layer of BiVO4,titanium dioxide(TiO_(2)) has been considered unsuitable because of its relatively positive valence band edge and low electrical conductivity.Herein,a crystal facet engineering of TiO_(2) nanostructures is proposed to control band structures for the hole blocking layer of BiVO4 nanodots.We design two types of TiO_(2) nanostructures,which are nanorods(NRs)and nanoflowers(NFs)with different(001)and(110)crystal facets,respectively,and fabricate BiVO4/TiO_(2) heterostructure photoanodes.The BiVO4/TiO_(2) NFs showed 4.8 times higher photocurrent density than the BiVO4/TiO_(2) NRs.Transient decay time analysis and time-resolved photoluminescence reveal the enhancement is attributed to the reduced charge recombination,which is originated from the formation of type II band alignment between BiVO4 nanodots and TiO_(2) NFs.This work provides not only new insights into the interplay between crystal facets and band structures but also important steps for the design of highly efficient photoelectrodes.
基金supported by National Natural Science Foundation of China(No.11175137)
文摘A large diamond crystal up to 500 μm in diameter with a smooth （100） facet at its top has been synthesized on Mo substrate through microwave plasma chemical vapor deposition （MPCVD）. Its morphology and quality were characterized by scanning electron microscopy （SEM）, and the growth mechanism was roughly illustrated from both macroscopic and microscopic viewpoints. It was found that morphological instabilities are a major factor resulting in synthesis of large diamond crystals, moreover, high microwave power density （MPD）, high CH4 concentrations, high pressure, high substrate surface temperature and the addition of a small amount of O2 were also necessary for the synthesis of large diamond crystals.
基金supported by the Natural Science Foundation of Hubei Province of China(2008CDB255)the Educational Commission of Hubei Province of China(No.Q20081505)the Key Laboratory for Green Chemical Process of the Ministry of Education of China (No.RGCT200801)
文摘A novel method was developed to deposit a large crystal diamond with good facets up to 1000 μm on a tungsten substrate using a microwave plasma enhanced chemical vapor deposition （MPCVD）. This method consists of two steps, namely single-crystal nucleation and growth. Prior to the fabrication of the well-faceted, large crystal diamond, an investigation was made into the nucleation and growth of the diamond which were affected by the O2 concentration and substrate temperature. Deposited diamond crystals were characterized by scanning electron microscopy and micro-Raman spectroscopy. The results showed that the conditions of single-crystal nucleation were appropriate when the ratio of H2/CH4/O2 was about 200/7.0/2.0, while the sub- strate temperature Ts of 1000℃ to 1050℃ was the appropriate range for single-crystal diamond growth. Under the optimum parameters, a well-faeeted large crystal diamond was obtained.
基金support from the National Natural Science Foundation of China(No.22005147)Dr.You acknowledges the financial support from the National Key Research and Development Program of China(2021YFA1600800)+1 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device(B21003)the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST),Ministry of Education(2021JYBKF03).
文摘The electrocatalytic water splitting technology can generate highpurity hydrogen without emitting carbon dioxide,which is in favor of relieving environmental pollution and energy crisis and achieving carbon neutrality.Electrocatalysts can effectively reduce the reaction energy barrier and increase the reaction efficiency.Facet engineering is considered as a promising strategy in controlling the ratio of desired crystal planes on the surface.Owing to the anisotropy,crystal planes with different orientations usually feature facet-dependent physical and chemical properties,leading to differences in the adsorption energies of oxygen or hydrogen intermediates,and thus exhibit varied electrocatalytic activity toward hydrogen evolution reaction(HER)and oxygen evolution reaction(OER).In this review,a brief introduction of the basic concepts,fundamental understanding of the reaction mechanisms as well as key evaluating parameters for both HER and OER are provided.The formation mechanisms of the crystal facets are comprehensively overviewed aiming to give scientific theory guides to realize dominant crystal planes.Subsequently,three strategies of selective capping agent,selective etching agent,and coordination modulation to tune crystal planes are comprehensively summarized.Then,we present an overview of significant contributions of facet-engineered catalysts toward HER,OER,and overall water splitting.In particular,we highlight that density functional theory calculations play an indispensable role in unveiling the structure–activity correlation between the crystal plane and catalytic activity.Finally,the remaining challenges in facet-engineered catalysts for HER and OER are provided and future prospects for designing advanced facet-engineered electrocatalysts are discussed.
基金the National Natural Science Foundation of China (U1632273, 21673214,U1732272, U1832165).
文摘This study investigated the positive effect of surface modification with ozone on the photocatalytic performance of anatase TiO2 with dominated (001) facets for toluene degradation. The performance of photocatalyst was tested on a home-made volatile organic compounds degradation system. The ozone modification, toluene adsorption and degradation mecha-nism were established by a combination of various characterization methods, in situ diuse reectance infrared fourier transform spectroscopy, and density functional theory calculation. The surface modtication with ozone can signiticantly enhance the photocatalytic degradation performance for toluene. The abundant unsaturated coordinated 5c-Ti sites on (001) facets act as the adsorption sites for ozone. The formed Ti-O bonds reacted with H2O to generate a large amount of isolated Ti5c-OH which act as the adsorption sites for toluene, and thus signi- cantly increase the adsorption capacity for toluene. The outstanding photo- catalytic performance of ozone-modified TiO2 is due to its high adsorption ability for toluene and the abundant surface hydroxyl groups, which produce very reactive OH· radicals under irradiation. Furthermore, the O2 generated via ozone dissociation could combine with the photogenerated electrons to form superoxide radicals which are also conductive to the toluene degradation.
文摘在KDP晶体（001）晶面上进行了四种压头（即：维氏压头、玻氏压头、圆锥压头、球形压头）的纳米压痕仿真研究。仿真结果表明：完全加载时四种压头与KDP晶体接触位置存在不同程度应力集中。当载荷在0-8 m N范围内时,其与等效应力影响深度呈近似线性递增关系。完全卸载时,残余应力分布深度为1.3-1.5μm。相同载荷条件下,各压头对应的塑性损伤层深度之间关系与等效应力影响深度之间关系一致。此外,通过纳米压痕实验验证了KDP晶体材料模型及相关参数的正确性。
基金supported by the National Natural Science Foundation of China(50625208,20773097,and 20877061)the National Basic Research Program of China(973Program,2007CB613302and2009CB939704)Fundamental Research Funds for the Central Universities(2010-YB-01)~~
基金National Natural Science Foundation of China(51172111,51402159)Shandong Province Higher Educational Science and Technology Program(J14LA17)+1 种基金China Postdoctoral Science Foundation(2015M57073)Qingdao Postdoctoral Application Research Project(2015116)。
