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基于密度泛函理论的NaTaO_(3)的结构设计及光催化抗菌性能研究
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作者 汪涛 张于浩 殷海荣 《人工晶体学报》 CAS 北大核心 2024年第6期1051-1060,共10页
NaTaO_(3)光催化剂因高的化学稳定性和热稳定性,以及环境友好性可以满足不同领域的需求。通过离子掺杂可以调节NaTaO_(3)的电子结构和性能,本文基于密度泛函理论研究了钙钛矿型Na_(0.75)B_(0.25)TaO_(3)(B=Cr,Mn,Fe,Cu,Zn)的电子结构和... NaTaO_(3)光催化剂因高的化学稳定性和热稳定性,以及环境友好性可以满足不同领域的需求。通过离子掺杂可以调节NaTaO_(3)的电子结构和性能,本文基于密度泛函理论研究了钙钛矿型Na_(0.75)B_(0.25)TaO_(3)(B=Cr,Mn,Fe,Cu,Zn)的电子结构和光学性质,分析了不同过渡金属掺杂对NaTaO_(3)的能带结构和电子态密度的影响。研究发现Cr、Mn、Fe和Zn掺杂使NaTaO_(3)呈现金属性质,Na_(0.75)Cu_(0.25)TaO_(3)则呈现半导体性质并且禁带宽度缩小到1.35 eV。掺杂Cu后会引起新的能级(Cu 3d和Cu 4s)在禁带中出现,这些新的能级位于禁带的中心,会导致禁带向导带移动。此外,Cu掺杂体系的吸收光谱发生了红移并且可将光吸收波长扩展到800 nm。接着,探索了NaTaO_(3)和Na_(0.75)Cu_(0.25)TaO_(3)的光催化抗菌性能,结果表明Cu离子调控后的光催化剂对金黄色葡萄球菌(S.aureus)的杀菌效率为99.99%,并对杀菌机理进行了分析。 展开更多
关键词 natao_(3) 密度泛函理论 过渡金属掺杂 电子结构 光学性质 光催化抗菌
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镧系元素(Ce、Pr、Nd、Sm、Eu)掺杂NaTaO_(3)光电性质影响的第一性原理研究 被引量:2
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作者 赵旭才 晋宇恒 +3 位作者 郭思嘉 卫来 张丽丽 雷博程 《电子元件与材料》 CAS 北大核心 2023年第9期1094-1101,共8页
为提高NaTaO_(3)在可见光区的光谱响应范围,利用第一性原理方法研究了镧系金属(Ce、Pr、Nd、Sm、Eu)掺杂NaTaO_(3)体系,并对掺杂前后体系的晶体结构、形成能、电子结构以及光学性质进行了计算与分析。结果表明:掺杂体系均发生了晶格畸变... 为提高NaTaO_(3)在可见光区的光谱响应范围,利用第一性原理方法研究了镧系金属(Ce、Pr、Nd、Sm、Eu)掺杂NaTaO_(3)体系,并对掺杂前后体系的晶体结构、形成能、电子结构以及光学性质进行了计算与分析。结果表明:掺杂体系均发生了晶格畸变,导致体系键布局发生变化,使体系内的正负电荷不再重合,从而在体系内产生了局域电势差,这有效阻碍了体系内部光生电子与空穴的复合,有利于提高NaTaO_(3)体系的光催化能力。在形成能的计算中发现NaTa_(0.875)Pr_(0.125)O_(3)的形成能最小,表明该体系最容易形成。掺杂体系的禁带宽度均减小,能级变密集。从态密度图中发现掺杂会加强原子轨道在费米能级的杂化程度,可以有效减少电子-空穴对的复合。从光学性质中发现Ce、Pr、Eu的掺入使NaTaO_(3)发生了红移,其中NaTa_(0.87)5Pr_(0.125)O_(3)对可见光的响应范围最广,该体系有望成为新型高效的光催化剂材料。 展开更多
关键词 natao_(3) 第一性原理 电子结构 光学性质 光催化
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Hydrothermal preparation of Nb-doped NaTaO_(3) with enhanced photocatalytic activity for removal of organic dye
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作者 Hao Zhou Qi Yin 《Chinese Journal of Chemical Engineering》 SCIE EI CAS CSCD 2022年第6期142-149,共8页
The construction of efficient photocatalysts has received much attention in wastewater treatment.In this study,Nb-doped NaTaO_(3) was prepared with different doping ratio by a facile hydrothermal method.The prepared c... The construction of efficient photocatalysts has received much attention in wastewater treatment.In this study,Nb-doped NaTaO_(3) was prepared with different doping ratio by a facile hydrothermal method.The prepared catalysts were analyzed by X-ray diffraction,scanning electron microscopy,Brunauer-EmmettTeller(BET)theory,ultraviolet–visible diffuse reflectance spectroscopy.Then the synthesized catalysts were employed to degrade a model pollutant,methylene blue(MB),under a 250 W mercury lamp.The characterization tests confirm that Nb was successfully doped into the crystal structure of NaTaO_(3) and the modified NaNb_(x)Ta_(1)·xO_(3)(x is the doping ratio;x=0.25,0.5,0.75)samples were formed,which were in regular cubic shapes just like pure NaTaO_(3).The synthesized NaNb_(x)Ta_(1)·xO_(3)(x=0.25,0.5,0.75)had improved specific surface area and narrowed band gaps compared with pure NaTaO_(3).In photocatalytic degradation experiments,NaNb0.75Ta0.25O_(3) presented the best photocatalytic activity ascribed to the narrow band gap and the high surface area,degradating 95.7%of MB after 180 min of reaction,which was even twice the ability of pure NaTaO_(3).Besides,the effects of possible inorganic anions and cations in wastewater on photocatalytic degradation were investigated.Electron spin resonance(ESR)tests and capture experiments were also conducted and a possible photocatalytic mechanism was proposed.This work provides a direction for constructing superior NaTaO_(3)-based photocatalysts to be widely utilized in environmental protection. 展开更多
关键词 Photocatalytic degradation Methylene blue natao_(3)
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Tunable bismuth doping/loading endows NaTaO_(3)nanosheet highly selective photothermal reduction of CO_(2) 被引量:3
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作者 Mengmeng Zhang Changhua Wang +3 位作者 Yueyun Wang Songmei Li Xintong Zhang Yichun Liu 《Nano Research》 SCIE EI CSCD 2023年第2期2142-2151,共10页
Photothermal CO_(2)reduction with H2O,integrating advantages of photocatalysis driven H2O splitting and thermal catalysis promoted CO_(2)reduction,has drawn sharply increasing attention in artificial synthesis of sola... Photothermal CO_(2)reduction with H2O,integrating advantages of photocatalysis driven H2O splitting and thermal catalysis promoted CO_(2)reduction,has drawn sharply increasing attention in artificial synthesis of solar fuels.The photothermal effect of metal nanoparticles facilities CO_(2)hydrogenation and activation of lattice oxygen in oxide photocatalyst promotes H2O oxidation,which is essentially considered for highly efficient photothermal catalysis.However,the large thermal conductivity of most metal nanoparticles induces inevitable heat dissipation,restricting the increase of catalyst temperature.In this work,to minimize the heat dissipation,we employ bismuth nanoparticles as photothermal unit,which is of the lowest thermal conductivity in the metal family.Meanwhile,we adopt bismuth doped NaTaO_(3)as photocatalytic unit because of the bismuth doping induced activation of lattice oxygen.The bismuth nanoparticles are assembled with bismuth doped NaTaO_(3)through one-step tunable transformation from Bi4TaO8Cl.Benefiting from the photothermal effect,thermal insulation caused by bismuth metal,and lattice oxygen activation by bismuth doping,the NaTaO_(3):Bi hybrid exhibits high photothermal catalytic performance.The yield of CO over NaTaO_(3):Bi hybrid at 413 K via photothermal catalysis is 141 times higher than that room temperature photocatalysis.Further,ultraviolet(UV)light irradiation leads to 89.2%selectivity of CO and visible light irradiation leads to 97.5%selectivity of CH4.This work may broaden the photocatalytic application of ABO_(3)perovskite and provides a novel strategy for the development of photothermal catalysts for artificial photosynthesis. 展开更多
关键词 CO_(2)reduction photothermal catalytic natao_(3) BISMUTH high selectivity
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Efficient degradation of organic pollutants by S-NaTaO_(3)/biochar under visible light and the photocatalytic performance of a permonosulfate-based dual-effect catalytic system 被引量:1
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作者 Yuehui Tai Jinlong Sun +6 位作者 Haoran Tian Fuyue Liu Boyu Han Wei Fu Zhangpei Liu Xiuye Yang Qifeng Liu 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2023年第3期388-400,共13页
Removing large concentrations of organic pollutants from water efficiently and quickly under visible light is essential to developing photocatalytic technology and improving solar energy efficiency.This study used a s... Removing large concentrations of organic pollutants from water efficiently and quickly under visible light is essential to developing photocatalytic technology and improving solar energy efficiency.This study used a simple hydrothermal method to prepare a non-metallic,S-doped NaTaO_(3)(S-NTO) photocatalyst,which was then loaded onto biochar (BC) to form a S-NTO/BC composite photocatalyst.After uniform loading onto BC,the S-NTO particles transformed from cubic to spherical.The photogenerated electron-hole pair recombination probability of the composite photocatalyst was significantly lower than those of the NTO particles.The light absorption range of the catalyst was effectively widened from 310 nm UV region to visible region.In addition,a dual-effect catalytic system was constructed by introducing peroxymonosulfate (PMS) into the environment of the pollution to be degraded.The Rhodamine B,Methyl Orange,Acid Orange 7,tetracycline,and ciprofloxacin degradation efficiency at 40 mg/L reached 99.6%,99.2%,84.5%,67.1%,and 70.7%,respectively,after irradiation by a 40 W lamps for 90 min.The high-efficiency visible-light catalytic activity of the dual-effect catalytic system was attributed to doping with non-metallic sulfur and loading of catalysts onto BC.The development of this dual-effect catalytic system provides new ideas for quickly and efficiently solving the problem of high-concentration organic pollution in aqueous environments,rationally and fully utilizing solar energy,and expanding the application of photocatalytic technology to practice. 展开更多
关键词 natao_(3) S-doped BIOCHAR Photocatalytic Permonosulfate Dual-effect catalytic system
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