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Oxygen vacancy-mediated WO_(3) phase junction to steering photogenerated charge separation for enhanced water splitting

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Journal of Advanced Ceramics 2022年第12期11卷 1873-1888页

作者： Huimin LI Qianqian SHEN Han ZHANG jiaqi GAO husheng jia Xuguang LIU Qi LI Jinbo XUE Key Laboratory of Interface Science and Engineering in Advanced Materials of Ministry of Education Taiyuan University of TechnologyTaiyuan 030024China Department of Chemistry Tsinghua UniversityBeijing 100084China College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030032China School of Materials Science and Engineering Southwest Jiaotong UniversityChengdu 610031China

Effective charge separation and transfer is deemed to be the contributing factor to achieve high photoelectrochemical(PEC)water splitting performance on *** a phase junction structure with controllable phase transition of WO_(3) can further improve the photocatalytic *** this work,we realized the transition from orthorhombic to monoclinic by regulating the annealing temperatures,and constructed an orthorhombic–monoclinic WO_(3)(o-WO_(3)/m-WO_(3))phase *** formation of oxygen vacancies causes an imbalance of the charge distribution in the crystal structure,which changes the W–O bond length and bond angle,accelerating the phase *** expected,an optimum PEC activity was achieved over the o-WO_(3)/m-WO_(3) phase junction in WO_(3)-450 photoelectrode,yielding the maximum O_(2) evolution rate roughly 32 times higher than that of pure WO_(3)-250 without any sacrificial agents under visible light *** enhancement of catalytic activity is attributed to the atomically smooth interface with a highly matched lattice and robust built-in electric field around the phase junction,which leads to a less-defective and abrupt interface and provides a smooth interfacial charge separation and transfer path,leading to improved charge separation and transfer efficiency and a great enhancement in photocatalytic *** work strikes out on new paths in the formation of an oxygen vacancy-induced phase transition and provides new ideas for the design of catalysts.

关键词： phase transition tungsten oxide lattice mismatch density functional theory(DFT) photoelectrocatalytic water splitting

Robust Fe^(2+)-doped nickel-iron layered double hydroxide electrode for electrocatalytic reduction of hexavalent chromium by pulsed potential method

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Journal of Materials Science & Technology 2022年第15期110卷 73-83页

作者： Zhifei Wang Jinbo Xue Yong Li Qianqian Shen Qi Li Xiaochao Zhang Xuguang Liu husheng jia Key Laboratory of Interface Science and Engineering in Advanced Materials Taiyuan University of TechnologyMinistry of EducationTaiyuan 030024China College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China School of Materials Science and Engineering Southwest Jiaotong UniversityChengdu 610031China College of Chemistry and Chemical Engineering Taiyuan University of TechnologyTaiyuan 030024China

Electrocatalytic reduction of Cr(Ⅵ)to less toxic Cr(Ⅲ)is deemed as a promising *** electrocatalytic reduction is always driven by a constant cathodic potential,which exhibits a repelling action to Cr(Ⅵ)oxyanions in wastewater and consequently suppresses reduction *** order to remarkably accelerate Cr(Ⅵ)electrocatalytic reduction,we applied a pulsed potential on an Fe^(2+)-NiFe LDH/NF electrode synthesized by in situ growth of Fe^(2+)-doped NiFe LDH nanosheets on Ni foam using a spontaneous redox *** anodic potential section,HCrO_(4)^(–) anions are adsorbed on the electrode surface and reduced to Cr(Ⅲ)by Fe^(2+).Then,Cr(Ⅲ)ions are desorbed from the electrode surface under coulombic *** regeneration of Fe^(2+) and direct reduction of Cr(Ⅵ)are achieved under cathodic potential *** pulsed potential can achieve complete elimination of Cr(Ⅵ)within 60 min at an initial concentration of 10 mg L^(-1),and the removal efficiency shows a 60%increase with respect to that under constant cathodic potential.

关键词： Hexavalent chromium Electrocatalytic reduction Pulsed potential NiFe LDH Fe cycle

Oxygen vacancy self-doped single crystal-like TiO_(2) nanotube arrays for efficient light-driven methane non-oxidative coupling

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Journal of Advanced Ceramics 2023年第8期12卷 1577-1592页

作者： Jinbo Xue Jinyu Li Zhe Sun Huimin Li Huan Chang Xuguang Liu husheng jia Qi Li Qianqian Shen Key Laboratory of Interface Science and Engineering in Advanced Materials Ministry of EducationTaiyuan University of TechnologyTaiyuan 030024China College of Materials Science and Engineering Taiyuan University of TechnologyTaiyuan 030024China Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering Taiyuan 030032China School of Materials Science and Engineering Southwest Jiaotong UniversityChengdu 610031China

Photocatalytic non-oxidative coupling of methane(PNOCM)is a mild and cost-effective method for the production of multicarbon ***,the separation of photogenerated charges and activation of methane(CH4)are the main challenges for this ***,single crystal-like TiO_(2) nanotubes(VO-p-TNTs)with oxygen vacancies(VO)and preferential orientation were prepared and applied to *** results demonstrate that the significantly enhanced photocatalytic performance is mainly related to the strong synergistic effect between preferential orientation and *** preferential orientation of VO-p-TNT along the[001]direction reduces the formation of complex centers at grain boundaries as the form of interfacial states and potential barriers,which improves the separation and transport of photogenerated ***,VO provides abundant coordination unsaturated sites for CH4 chemisorption and also acts as electron traps to hinder the recombination of electrons and holes,establishing an effective electron transfer channel between the adsorbed CH4 molecule and photocatalyst,thus weakening the C–H *** addition,the introduction of VO broadens the light absorption *** a result,VO-p-TNT exhibits excellent PNOCM performance and provides new insights into catalyst design for CH4 conversion.

关键词： TiO_(2)nanotubes(TNTs) oxygen vacancies(VO) preferential orientation photocatalytic non-oxidative coupling of methane(PNOCM)

氨氧化Pt-Rh-Pd合金组合网催化剂（英文）

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稀有金属材料与工程 2017年第2期46卷 339-343页

作者：刘欣韩勇强贾虎生太原理工大学山西太原030024 中海油太原贵金属有限公司山西太原030006

通过研究氨氧化用Pt-Rh-Pd合金网催化剂,旨在为了提高工业硝酸生产的效率。按照氧化炉中氨氧化反应的特性,将该催化剂分为3个反应区域。Pt-Rh-Pd合金组合网催化剂安装在氨氧化双加压机组中,其直径3880 mm、操作压力0.35 MPa。根据FESEM... 详细信息

通过研究氨氧化用Pt-Rh-Pd合金网催化剂,旨在为了提高工业硝酸生产的效率。按照氧化炉中氨氧化反应的特性,将该催化剂分为3个反应区域。Pt-Rh-Pd合金组合网催化剂安装在氨氧化双加压机组中,其直径3880 mm、操作压力0.35 MPa。根据FESEM和EDS对表面形貌的研究,提出了催化网的反应机理。通过氧化率计算,使用Pt-Rh-Pd合金组合网氧化率提高了1%。Pd的掺入使催化剂兼具催化、捕集、固溶和再催化的作用。同时,采购成本降低30%,Pt损耗由120 mg降低至70 mg。因此,该催化剂具有广泛的应用前景。

关键词： Pt-Rh-Pd合金组合网催化剂氨氧化

Pd纳米颗粒协同氧空位增强TiO_(2)光催化CO_(2)还原性能

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无机材料学报 2023年第11期38卷 1301-1308页

作者：贾鑫李晋宇丁世豪申倩倩贾虎生薛晋波太原理工大学新材料界面科学与工程教育部重点实验室太原030024 太原理工大学材料科学与工程学院太原030024

针对TiO_(2)表面活性位点不足、反应动力学缓慢、CO_(2)还原产物中碳氢化合物的产率低以及选择性差等问题,研究通过Pd催化氧还原法在缺氧环境中构筑了具有表面氧空位的一维单晶TiO_(2)纳米带阵列(Pd-Ov-TNB)。通过形貌结构、载流子行为... 详细信息

针对TiO_(2)表面活性位点不足、反应动力学缓慢、CO_(2)还原产物中碳氢化合物的产率低以及选择性差等问题,研究通过Pd催化氧还原法在缺氧环境中构筑了具有表面氧空位的一维单晶TiO_(2)纳米带阵列(Pd-Ov-TNB)。通过形貌结构、载流子行为及光催化性能分析,探究了表面氧空位和Pd的氢溢流效应对光生载流子分离传输及还原产物选择性的影响。结果表明,Pd-Ov-TNB的CO_(2)还原活性强,产物中CH_(4)、C_(2)H_(6)和C_(2)H_(4)的产率分别为40.8、32.09和3.09μmol·g^(–1)·h^(–1),碳氢化合物的选择性高达84.52%,在C–C偶联方面展现出巨大的潜力。其一维单晶纳米带结构提高了材料的活性比表面积和结晶度,为CO_(2)还原反应提供了更多的活性位点,并加速载流子的分离传输。同时,氧空位增强了光生电荷的表面积累,为CO_(2)还原提供了富电子环境。此外,Pd纳米颗粒提高反应体系中H^(*)的浓度,并通过氢溢流效应将H*转移到催化剂表面吸附CO_(2)的活性位点,促进反应中间产物氢化。各种优势共同作用促使CO_(2)向碳氢化合物高效转化。

关键词：氧空位 TiO_(2)纳米带氢溢流光催化还原CO_(2)

Pd增强缺陷态TiO_(2)纳米管阵列的光催化产氢性能

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高等学校化学学报 2022年第10期43卷 92-100页

作者：姜珊申倩倩李琦贾虎生薛晋波太原理工大学新材料界面科学与工程教育部重点实验室太原030024 清华大学化学系北京100084 太原理工大学材料科学与工程学院太原030024 西南交通大学材料科学与工程学院成都610031

通过光还原沉积法,利用氧空位诱导作用,在Ni掺杂的缺陷态TiO_(2)纳米管阵列(TNT-Ni)上得到金属Pd含量不同的Pd-TNT-Ni催化剂.采用场发射扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、紫外-可见漫反射(UV-Vis DRS)、表面光电压(SPV)、光... 详细信息

通过光还原沉积法,利用氧空位诱导作用,在Ni掺杂的缺陷态TiO_(2)纳米管阵列(TNT-Ni)上得到金属Pd含量不同的Pd-TNT-Ni催化剂.采用场发射扫描电子显微镜(SEM)、X射线光电子能谱(XPS)、紫外-可见漫反射(UV-Vis DRS)、表面光电压(SPV)、光致发光光谱(PL)和电化学测试等表征手段,探究了Pd与Ni掺杂的缺陷态TiO_(2)纳米管阵列之间的强相互作用对其光吸收特性和载流子分离及传输效率的影响,阐明了强相互作用对材料光催化活性的调控机理,提出了Pd增强Pd-TNT-Ni光催化性能的作用机理.结果表明,通过光还原法制备的Pd纳米颗粒尺寸为10~20 nm的Pd_(120)-TNT-Ni样品的光响应值为4.22 mA/cm^(2),是未负载Pd样品光响应值(1.14 mA/cm^(2))的3.7倍,其具有最佳的平均产氢速率(5.16 mmol·g^(‒1)·h^(‒1)),是TNT样品平均产氢速率(0.45 mmol·g^(‒1)·h^(‒1))的12倍,表明Pd与缺陷态TiO_(2)纳米管阵列之间的强相互作用驱动了载流子的分离及传输,且Pd作为电子捕获势阱及反应活性位点,显著提高了材料的光催化性能.

关键词：氧空位钯负载金属载体间强相互作用缺陷态二氧化钛纳米管阵列光催化产氢

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纳米氧化铝粉体的制备

金刚石与磨料磨具工程 2005年第2期25卷 61-63页

作者：司文元裴小苗贾虎生许并社太原理工大学材料科学与工程学院太原030024

溶胶-凝胶法是目前在氧化物纳米粉制备中研究和应用较多的一种方法。但多数研究集中在用各种昂贵的有机醇盐作前驱体制备纳米氧化铝粉。本实验研究用廉价的AlCl3·6H2O作原料探索一种制备纳米氧化铝粉的可行的方法。以期能为纳米氧化铝... 详细信息

溶胶-凝胶法是目前在氧化物纳米粉制备中研究和应用较多的一种方法。但多数研究集中在用各种昂贵的有机醇盐作前驱体制备纳米氧化铝粉。本实验研究用廉价的AlCl3·6H2O作原料探索一种制备纳米氧化铝粉的可行的方法。以期能为纳米氧化铝的大量应用提供可能。通过实验优化了凝胶制备过程的的主要参数(铝离子浓度、反应物配比、反应温度、添加剂),制得了稳定的凝胶。在1150℃(1.5h)的条件下制得了粒径为10纳米左右的α-Al2O3粉体。

关键词：溶胶-凝胶法氧化铝纳米粉体

Synthesis and luminescent properties of terbium complex containing 4-benzoylbenzoic acid for application in NUV-based LED

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Journal of Rare Earths 2016年第2期34卷 130-136页

作者：孙乃群赵希瑾杨亚敏李利平张爱琴贾虎生刘旭光 Key Laboratory of Interface Science and Engineering in Advanced Materials of Taiyuan University of Technology Ministry of Education College of Materials Science and Engineering Taiyuan University of Technology College of Textile Engineering Taiyuan University of Technology College of Chemistry and Chemical Engineering Taiyuan University of Technology

A novel Tb(III) ternary complex Tb(p-BBA)3MAA was synthesized with 4-benzoylbenzoic acid (p-BBA) and methacrylic acid (MAA) as ligands. The complex was characterized by IR, UV-visible, thermogravimetric analysis and fluorescence spectroscopy. Monitored at 544 nm, the complex displayed wide and strong excitation band at 300–400 nm, which matched well with the 365 nm-emitting UV chip. The complex exhibited excellent green emission at 544 nm (5D4→7F5 transition of Tb3+) under an excitation at 365 nm. Besides, the complex showed high thermal stability. Its intramolecular energy transfer process was further discussed. Fur-thermore, the complex also had higher fluorescence lifetime (1.38 ms) and higher quantum yield (0.372). Finally, electroluminescent properties indicated that when used to fabricate LED with 365 nm UV chip (power efficiency is 18.6 lm/W), the complex remained its favorable optical performance. These results implied that Tb(p-BBA)3MAA could be used as a green phosphor for NUV-based white LED.

关键词： 4-benzoylbenzoic acid Tb(III) complex fluorescence quantum yield lifetime rare earths

Mo原子嵌入对C_(36)结构和性能的影响

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材料研究学报 2006年第4期20卷 431-434页

作者：王丽平韩培德贾虎生许并社太原理工大学材料科学与工程学院太原030024

用密度泛函方法采用GGA／PW91基组对具有D6h对称性的C36及其衍生物Mo@C36进行结构优化和性能计算,研究Mo@C36稳定构型、存在的可能性及稳定性,以及Mo掺杂对C36结构及性能的影响．结果表明,Mo位于C36主轴上偏离中心约0．1 nm时,M0@C36能... 详细信息

用密度泛函方法采用GGA／PW91基组对具有D6h对称性的C36及其衍生物Mo@C36进行结构优化和性能计算,研究Mo@C36稳定构型、存在的可能性及稳定性,以及Mo掺杂对C36结构及性能的影响．结果表明,Mo位于C36主轴上偏离中心约0．1 nm时,M0@C36能量最低,结构最稳定;Mo掺杂引起笼的局部畸变,但Mo@C36仍保持完整笼型结构,其稳定性比C36有所提高．Mo原子嵌入C36使其禁带宽度增大,导电性及化学反应活性降低;费米能级下降,但仍处于禁带之间,二者均属半导体性质的材料．C36结构及性能的变化与Mo所处的位置及Mo与C36笼之间的电子迁移有关．

关键词：材料科学基础学科 Ca6 Mo@C36 密度泛涵电子结构