Synergistic effect of N- and F-codoping on the structure and photocatalytic performance of TiO2

Three types of TiO₂ nanostructures were synthesized via a facile hydrolysis method at 195 °C. Effects of the preparation method and doping with N and F on the crystal structure and photocatalytic performance of TiO₂ were investigated. The nanomaterials were characterized by X-ray diffraction, transmission electron microscopy, X-ray photoelectron spectroscopy, Brunauer–Emmett–Teller porosimetry, ultraviolet–visible diffuse reflectance spectroscopy and fluorescent emission spectra. Their photo-catalytic activity was examined by the photodegradation of methylene blue in aqueous solution under both ultra-violet and visible light irradiation. The results show that nitrogen and fluorine co-doped anatase TiO₂ had the characteristics of a smaller crystalline size, broader light absorption spectrum and lower charge recombination than pure TiO₂. Most importantly, more efficient photocatalytic activity under both ultra-violet and visible light was observed. The obtained N–F-TiO₂ nanomaterial shows considerable potential for water treatment under sunlight irradiation.     

利用碳氮共掺杂二氧化钛纳米管阵列实现同时降解甲基橙和产氢

本研究结合阳极氧化和超声辅助沉积的方法合成碳氮共掺杂的二氧化钛纳米管阵列,并采用XRD、FESEM、UV-vis、XPS等技术对材料进行表征.光电化学(PEC)体系中,碳氮共掺杂二氧化钛纳米管阵列作为阳极,甲基橙溶液作为光电催化氧化的对象,对光催化剂的氧化性能进行了考察,与此同时,在阴极实现光解水产氢,最终在PEC体系中实现同时降解甲基橙和产氢.XRD、FESEM、UV-vis、XPS及TEM等表征结果表明,碳氮成功地掺入到了二氧化钛纳米管阵列中,并未破坏其多孔有序的结构,而且比二氧化钛纳米管阵列具有更高的光催化活性.光电催化降解甲基橙的实验当中,在酸性溶液条件下,二氧化钛纳米管阵列的催化氧化效率较高,降解效率达到了100%,其速率常数为2.3×10-3s-1(p H=4),同时也具有较高的产氢速率(0.95 mmol·h-1),因此,该实验体系在光电催化降解污水中的有机污染物同时产氢方面有应用前景.     

熔盐法制备K+-g-C3N4及其光催化降解有机污染物性能

采用熔盐法制备了能级位置可控的钾离子掺杂石墨相氮化碳催化剂（g-C₃N₄）,并考察了其在可见光下降解罗丹明B（RhB）性能.采用XRD、UV-Vis、XPS、N₂吸附、PL、EIS等手段对催化剂进行了表征.结果表明,钾离子的引入降低了催化剂粒径尺寸,提高了比表面积,改善了光生电子-空穴对的分离效率.不仅如此,通过控制钾离子掺杂量可以实现催化剂的能级位置在一定范围内的任意调变,使有机污染物的氧化降解反应从·O₂^-单一氧化剂反应变成·OH和·O₂^-双氧化剂反应,大大提高了降解率.制备的钾离子掺杂g-C₃N₄的RhB降解速率常数达到0.022min^-1,是纯g-C₃N₄的5倍.不仅如此,通过对能级位置的调控,制备的催化剂对其他多种有机污染物如甲基蓝,苯酚等的降解率也有显著提高.     

Sb2O5/TiO2催化超声降解甲基橙溶液

采用实验室合成的Sb2O5掺杂TiO2作为催化剂,研究各种因素对甲基橙的超声催化降解反应的影响.结果表明,在Sb2O5掺杂TiO2催化剂作用下,甲基橙的超声催化降解效果明显优于单独使用TiO2的情况.1.5%掺杂量的催化剂,用量在1.0～1.5 g/L之间,超声波频率25 kHz,输出功率1.0 W/cm2,pH为1.0～3.0时,初始浓度为20 mg/L的甲基橙水溶液,100 min左右基本可全部降解,COD去除率达到99.0%以上.Sb2O5掺杂TiO2催化超声降解有机污染物的方法具有很好的应用前景.     

同步活化氮掺杂海藻酸钠基多孔碳制备及对双酚A的高效吸附

为了进一步提升多孔碳材料的吸附性能,以海藻酸钠(SA)为碳前驱体、K2CO3为活化剂、三聚氰胺为氮掺杂剂,通过一步法实现同步活化氮掺杂海藻酸钠基多孔碳材料(SAC/N)的制备,研究了掺氮比对多孔碳吸附性能的影响.采用扫描电子显微镜(SEM)、X射线衍射仪(XRD)、X射线光电子能谱仪(XPS)等方法对样品进行了表征.结...     

掺硼铁氧化物在紫外-可见光下的催化性能

采用溶胶凝胶法制备不同掺硼量的针铁矿和赤铁矿催化剂,并用X射线衍射图谱（XRD）、比表面积（BET法）、紫外可见漫反射光谱（DRS）及电荷零点（盐滴定法）对催化剂进行表征.结果表明：硼掺杂能改变催化剂的晶体结构,增大其比表面积和Lewis表面酸度,并能提高催化剂的紫外-可见光活性.在紫外光下,掺硼质量分数2%的赤铁矿对...     

可见光响应手性TiO2复合光催化剂及其降解有机污染物

通过空穴和自由基捕获剂的加入,首先研究了可见光激发下手性TiO₂复合光催化剂降解罗丹明B和四环素的机理. 结果表明,可见光激发TiO₂光催化剂降解罗丹明B和四环素的机理是相同的,其形成的光生空穴是降解有机物的关键影响因素.利用D型手性表面活性剂在低温时可以构建右旋非对称手性堆积结构的D-TiO₂. 这种非对称结构在介孔TiO₂内部引入氧空穴和Ti-N键,使D-TiO₂也具有显著的可见光响应和可见光降解活性. La³⁺ 或者Fe³⁺的掺杂几乎不影响催化剂的形貌及其TiO₂的结晶过程, 但可以在催化剂中形成光生空穴和电子的捕获中心,显著提升可见光激发下TiO₂催化剂中光生空穴和电子的分离率,从而增强催化剂对四环素的光降解活性.     

γ-Fe2O3抗As2O3中毒能力的分子模拟

采用密度泛函理论研究了γ-Fe₂O₃表面As₂O₃的吸附以及掺杂改性提高抗As₂O₃中毒性能的作用机理.计算了As₂O₃在完整以及O缺陷γ-Fe₂O₃（001）表面的吸附性能,包括吸附位点、吸附结构、吸附能、PDOS等.同时建立了Mo、Ti、Mg掺杂的γ-Fe₂O₃模型,探讨了助剂掺杂对抗砷中毒能力的作用机制,并考虑了掺杂量的影响.结果表明：As₂O₃倾向于以O端化学吸附在γ-Fe₂O₃（001）表面Fe_oct位,吸附过程发生强烈的相互作用和电荷转移.当表面存在O缺陷时,As₂O₃的吸附能得到提高.Mo、Ti、Mg倾向于掺杂在Fe_oct位,增强了对As₂O₃的吸附能力,并且增大Mo的掺杂量可以强化As₂O₃的吸附.As₂O₃倾向于与活性较强的Mo、Ti、Mg发生反应,从而保护活性Fe位不受砷中毒,Ti和Mg的掺杂还抑制了相邻Fe位对As₂O₃的吸附.Mo、Ti、Mg的掺杂还促进了催化剂表面对NH₃的吸附,增强了表面酸性强度,有利于SCR反应.Mo、Ti、Mg原子的掺杂有利于提高γ-Fe₂O₃催化剂的抗砷中毒性能.     

脯氨酸掺杂g-C3N4纳米片的制备及其对RhB的降解

通过简单的水热及煅烧方法制备了脯氨酸掺杂的g-C₃N₄纳米片,借助FTIR、XRD、SEM、BET、XPS、UV-vis DRS、PL、电化学工作站等手段对所制备的光催化剂进行结构、形貌、组成及光电性能表征分析.结果表明,脯氨酸的加入可以自主剥离前驱体,制成纳米片状的g-C₃N₄,增加催化剂的比表面积.此外脯氨酸的引入可以调节催化剂的能带结构,增加可见光吸收,提高光生载流子分离率.在模拟可见光照射下,考察其对罗丹明B (RhB)的光催化降解性能获得了最优掺杂条件.1%脯氨酸掺杂(PCN-1%)的催化剂经过60min可见光照射即可降解99%以上的污染物.降解速率得到显著提升,PCN-1%对RhB的降解速度(0.0271min^-1)达到传统体相氮化碳(BCN)降解速率(0.0027min^-1)的10.04倍,显著提高了g-C₃N₄的光催化能力.     

N-doped CoAl oxides from hydrotalcites with enhanced oxygen vacancies for excellent low-temperature propane oxidation

A series of nitrogen-doped CoAlO (N-CoAlO) were constructed by a hydrothermal route combined with a controllable NH₃ treatment strategy. The effects of NH₃ treatment on the physico-chemical properties and oxidation activities of N-CoAlO catalysts were investigated. In comparison to CoAlO, a smallest content decrease in surface Co³⁺ (serving as active sites) while a largest increased amount of surface Co²⁺ (contributing to oxygen species) are obtained over N-CoAlO/4h among the N-CoAlO catalysts. Meanwhile, a maximum N doping is found over N-CoAlO/4h. As a result, N-CoAlO/4h (under NH₃ treatment at 400°C for 4 hr) with rich oxygen vacancies shows optimal catalytic activity, with a T₉₀ (the temperature required to reach a 90% conversion of propane) at 266°C. The more oxygen vacancies are caused by the co-operative effects of N doping and suitable reduction of Co³⁺ for N-CoAlO/4h, leading to an enhanced oxygen mobility, which in turn promotes C₃H₈ total oxidation activity dominated by Langmuir-Hinshelwood mechanism. Moreover, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTs) analysis shows that N doping facilities the decomposition of intermediate species (propylene and formate) into CO₂ over the catalyst surface of N-CoAlO/4h more easily. Our reported design in this work will provide a promising way to develop abundant oxygen vacancies of Co-based catalysts derived from hydrotalcites by a simple NH₃ treatment.