碳量子点掺杂氮化碳提高的光电化学阴极保护性能研究

目的研究g-C_3N_4/C-Dots-M复合材料的光电化学阴极保护性能。方法采用X射线衍射(XRD)、扫描电子显微镜(SEM)和紫外可见漫反射光谱技术对样品的晶体结构、微观形貌和光吸收性能进行表征。通过电化学测试可见光照射下g-C_3N_4/C-Dots-M复合材料光电极偶联316L不锈钢后的光电化学阴极保护电流密度和电位变化曲线,研究材料的光电化学阴极保护性能。结果可见光照射下,该偶联体系的光致混合电位下降至-0.43 V(vs. Ag/AgCl),光电化学阴极保护电流密度达到4.3μA/cm。结论得益于碳量子点优异的电子传导特性,g-C_3N_4/C-Dots-550复合材料的光电化学阴极保护性能比纯g-C_3N_4的明显增强。该复合材料在光电化学阴极保护方面展现了较大的应用潜力。     

Fabrication and photoelectrocatalytic properties of nanocrystalline monoclinic BiVO4 thin-film electrode

Monoclinic bismuth vanadate(BiVO4) thin film was fabricated on indium-tin oxide glass from an amorphous heteronuclear complex via dip-coating.After annealation at 400,500,and 600°C,the thin films were characterized by X-ray diffraction,field emission scanning electron microscopy,X-ray photoelectron spectroscopy,and UV-Vis spectrophotometry.The BiVO4 particles on the ITO glass surface had a monoclinic structure.The UV-Visible diffuse reflection spectra showed the BiVO4 thin film had photoabsorption propertie...     

微生物光电化学池去除硝酸盐氮:以PANI/TiO2-NTs为光阳极

利用微生物光电化学池(MPEC)去除污染物是一种经济高效环保的方法.本实验在制备获得聚苯胺/二氧化钛纳米管阵列(PANI/TiO_2-NTs)复合光电极的基础上,构建了由PANI/TiO_2-NTs光阳极和生物阴极组成的MPEC系统,并对其去除硝酸盐氮(NO~-_3-N)的性能进行研究.结果表明,PANI负载时间为80 s时,PANI/TiO_2-NTs电极光电性能最佳,相比于TiO_2-NTs电极光电流密度增大约一倍,PANI的修饰有效提高了光能利用率.构建的MPEC系统能在无外加电压的条件下利用光能驱动实现自养反硝化脱氮,NO~-_3-N的生物降解符合准一级反应动力学方程.光响应电流密度越大,系统反硝化脱氮性能越好,NO~-_3-N初始浓度为25 mg·L~(-1)时,当光响应电流密度从0.17 mA·cm~(-2)增加至0.67 mA·cm~(-2),平均反硝化速率从0.83 mg·(L·h)~(-1)增大到2.83 mg·(L·h)~(-1).对生物阴极微生物膜进行了高通量测序,发现Pseudomonas所占比例最大(27.37%)为优势菌属.分析认为PANI/TiO_2-NTs光阳极产生的光生电子通过外电路传递到阴极,Pseudomonas、Alishewanella和Flavobacterium等具有自养反硝化能力和电化学活性的微生物可直接利用电极上的电子作为唯一的电子供体进行自养反硝化脱氮.     

Electrically enhanced photodegradation of an azodye(Acid Orange II) using a Pt/TiO_2 film electrode irradiating with an UV lamp

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Electrically enhanced photodegradation of an azodye(Acid Orange Ⅱ) using a Pt/TiO2 film electrode irradiating with an UV lamp

A photoelectrochemical process in the degradation of an azodye(Acid Orange II)on a Pt/TiO2 film electrode was investigated.By using the glass device and the voltage stabilized source of direct current,decolorization ratios higher than 78% were observed during a period of 5h.Comparing this value with the sum of the decolorization ratios obtained by a sole application of electrochemical(lower than 3%)and photochemical(about 23%)procedures, a significant synergic effect between both processes was observed.The effects of adscititious voltage and pH value on the decolorization ratios were obvious while the effect of the amount of aeration was minor.     

BiVO4-Cu2O/CuO双光电极自偏压光电催化降解苯酚研究

基于费米能级差,构建了以BiVO_4为光阳极,Cu_2O/CuO为光阴极的双光电极可见光响应光催化燃料电池体系,研究了该体系在不同氧化剂的辅助作用下光电催化降解苯酚的效率与动力学.结果表明,向该体系中投加H_2O_2可以显著促进苯酚的降解,且反应过程光电流稳定,铜溶出量低.详细探究了H_2O_2初始浓度、pH对降解的影响,结果表明在H_2O_2投加量为5 mmol·L~(-1),初始pH为3.5条件下利于苯酚降解,5 mg·L~(-1)的苯酚可在120 min内完全去除.顺磁共振和猝灭实验表明该体系的主要氧化物种为·OH、·O~-_2和光生空穴.该催化体系实现了苯酚在可见光下的高效催化降解.     

光电化学阴极保护的原理及研究进展

简要介绍了光电化学阴极保护技术的基本原理以及其影响因素,总结了历年来该方面的主要研究成果,并简要地介绍了笔者课题组在光电化学阴极保护方面的部分工作。最后,对光电化学阴极保护技术进一步的发展以及应用进行了展望。     

Photoelectrochemical degradation of Methylene Blue with -PbO2 electrodes driven by visible light irradiation

-PbO2 electrodes were prepared by electro-deposition and characterized by scanning electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and linear sweep voltammetry. We confirmed pure -PbO2 crystals were on the electrode and it had a high oxygen evolution potential. The photoactivity and photoelectrochemical (PEC) properties of the -PbO2 electrode were investigated under visible light irradiation ( > 420 nm) for the decolorization of Methylene Blue. Pseudo first-order kinetics parameter (Kapp) for dye decolorization using the -PbO2 electrode achieved 6.71×10?4 min?1 under visible light irradiation, which indicated its excellent visible light-induced photoactivity. The Kapp of the PEC process was as much as 1.41×10?3 min?1 and was 1.71 times that of visible light irradiation or electrolysis even in the presence of the -PbO2 electrode. A significant synergetic effect was observed in the PEC system. We also employed TiO2 modified -PbO2 electrodes in this test, which revealed that the TiO2 immobilized on the -PbO2 electrode inhibited the visible light-induced PEC efficiency despite the amount of TiO2 used for electrode preparation. The -PbO2 electrode was also superior to the dimensionally stable anode (Ti/Ru0:3Ti0:7O2) in visible light-induced photoactivity and PEC efficiency.     

苯乙烯致DNA间接损伤效应的光电化学生物传感器快速检测

许多有机化合物自身没有致癌毒性,但进入生物体内,经过体内代谢酶的催化后转化成活性中间体,与DNA形成共价化合物.这些间接的损伤会最终导致DNA分子结构和功能的变化,对人类的健康造成威胁.因此,建立一种快速有效的方法检测间接致癌化合物对DNA的损伤,成为当前研究的热点.论文建立了一种新型的光电化学生物传感器来检测有机化合物苯乙烯对DNA的间接损伤效应,该传感器以层层自组装的方式将光电信号分子、双链DNA和血红蛋白组装在半导体电极上.在H2O2存在的条件下,传感膜中的血红蛋白可将苯乙烯转化为氧化苯乙烯,氧化苯乙烯扩散到膜内,与DNA形成加合物,引起DNA结构变化,导致光电分子光电流信号的增加.实验中,将修饰好的电极置于终浓度为2mM H2O2和2%苯乙烯(体积比)的混合液(pH7.3的磷酸缓冲液配制)中反应一段时间后,在电解质溶液中进行光电流检测.实验结果表明,光电流信号随着反应时间逐渐升高,在30min后趋于稳定,表明苯乙烯在传感膜上的氧化和DNA的损伤反应基本完成.与反应前相比,反应后光电流增加了40%,并且酶催化苯乙烯生成的氧化苯乙烯经紫外可见光谱得到验证.论文建立的光电化学生物传感器模拟了体内DNA损伤反应过程,能快速有效地检测苯乙烯对DNA的间接损伤效应,有望为有机化合物潜在基因毒性的风险评估提供一个快速筛查工具。     

Wastewater treatment meets artificial photosynthesis: Solar to green fuel production,water remediation and carbon emission reduction

• Mitigating energy utilization and carbon emission is urgent for wastewater treatment. • MPEC integrates both solar energy storage and wastewater organics removal. • Energy self-sustaining MPEC allows to mitigate the fossil carbon emission. • MPEC is able to convert CO₂ into storable carbon fuel using renewable energy. • MPEC would inspire photoelectrochemistry by employing a novel oxidation reaction. Current wastewater treatment (WWT) is energy-intensive and leads to vast CO₂ emissions. Chinese pledge of “double carbon” target encourages a paradigm shift from fossil fuels use to renewable energy harvesting during WWT. In this context, hybrid microbial photoelectrochemical (MPEC) system integrating microbial electrochemical WWT with artificial photosynthesis (APS) emerges as a promising approach to tackle water-energy-carbon challenges simultaneously. Herein, we emphasized the significance to implement energy recovery during WWT for achieving the carbon neutrality goal. Then, we elucidated the working principle of MPEC and its advantages compared with conventional APS, and discussed its potential in fulfilling energy self-sustaining WWT, carbon capture and solar fuel production. Finally, we provided a strategy to judge the carbon profit by analysis of energy and carbon fluxes in a MPEC using several common organics in wastewater. Overall, MPEC provides an alternative of WWT approach to assist carbon-neutral goal, and simultaneously achieves solar harvesting, conversion and storage.