Bi/BiOI可见光催化氧化去除NO的性能

催化机理是催化反应过程中的一大重要问题。为研究可见光催化氧化去除NO的反应机理,提高大气中NO去除效率,将BiOI中的Bi 3+部分还原为金属Bi沉积在BiOI纳米片表面,合成Bi/BiOI纳米级微球光催化剂。通过一系列表征分析发现,金属Bi沉积在BiOI表面后,催化剂的微观结构和光学性质都有明显变化。与纯相的BiOI相比,制备的Bi/BiOI催化剂对气态NO表现出更优异的可见光催化去除活性。通过金属Bi的表面等离子体共振,引起高效可见光吸收和电子空穴对分离。同时,运用原位红外光谱动态监测Bi/BiOI光催化氧化NO的反应过程,结合自由基捕获结果,从分子层面揭示其反应产物,并结合表面等离子体共振提出Bi/BiOI光催化作用机理。

路表径流冲刷过程中透水沥青道路的污染物释放与截留特性研究

海绵城市的兴起使透水性机动车道路的需求大增.一方面,传统的沥青道路修建材料中含大量可挥发和可淋溶的有机物,在修建和使用过程中可能污染环境;另一方面,透水沥青道路为多孔结构,在使用中可能对下渗经过的路表径流中的污染物有吸附截留作用.为明确这两方面的规律,本文以苯酚和铅为研究对象,研究了新建沥青道路的污染物释放规律和使用中沥青道路对路表径流中污染物的截留作用.结果表明,新建沥青道路在路表径流下渗淋溶过程中有大量苯酚释放,而重金属铅没有检出;使用中的沥青道路对下渗经过的苯酚和重金属铅有一定的截留作用.因此,在沥青道路设计和施工中,应有针对性的改善材料成分和道路结构,以减少本身污染物的释放并加强对污染物的截留作用.

Synergistic integration of metallic Bi and defects on BiOI: Enhanced photocatalytic NO removal and conversion pathway

Surface plasmon resonance(SPR)of metals may provide a way to improve light absorption and utilization of semiconductors,achieving better solar light conversion and photocatalysis efficiency.This study uses the advantages of SPR in metallic Bi and artificial defects to cooperatively enhance the photocatalytic performance of BiOI.The catalysts were prepared by partial reduction of BiOI to form Bi@defective BiOI,which showed highly enhanced visible photocatalytic activity for NOx removal.The effects of reductant quantity on the photocatalytic performance of Bi@defective BiOI were investigated.The as-prepared photocatalyst(Bi/BiOI-2)using 2 mmol of reductant NaBH4 showed the most efficient visible light photocatalytic activity.This enhanced activity can be ascribed to the synergistic effects of metallic Bi and oxygen vacancies.The electrons from the valence band tend to accumulate at vacancy states;therefore,the increased charge density would cause the adsorbed oxygen to transform more easily into superoxide radicals and,further,into hydroxyl radicals.These radicals are the main active species that oxidize NO into final products.The SPR effect of elemental Bi enables the improvement of visible light absorption efficiency and the promotion of charge carrier separation,which are crucial factors in boosting photocatalysis.NO adsorption and reaction processes on Bi/BiOI-2 were dynamically monitored by in situ infrared spectroscopy(FT-IR).The Bi/BiOI photocatalysis mechanism co-mediated by elemental Bi and oxygen vacancies was proposed based on the analysis of intermediate products and DFT calculations.This present work could provide new insights into the design of high-performance photocatalysts and understanding of the photocatalysis reaction mechanism for air-purification applications.

A Bi/BiOI/(BiO)_2CO_3 heterostructure for enhanced photocatalytic NO removal under visible light

Narrow-band BiOI photocatalysts usually suffer from low photocatalysis efficiency under visible light exposure because of rapid charge recombination. In this work, to overcome this deficiency of photosensitive BiOI, oxygen vacancies, Bi particles, and Bi2O2CO3 were co-induced in BiOI via a facile in situ assembly method at room temperature using NaBH4 as the reducing agent. In the synthesized ternary Bi/BiOI/(BiO)2CO3, the oxygen vacancies, dual heterojunctions (i.e., Bi/BiOI and Bi- OI/(BiO)2CO3), and surface plasmon resonance effect of the Bi particles contributed to efficient electron-hole separation and an increase in charge carrier concentration, thus boosting the overall visible light photocatalysis efficiency. The as-prepared catalysts were applied for the removal of NO in concentrations of parts per billion from air in continuous air flow under visible light illumination. Bi/BiOI/(BiO)2CO3 exhibited a highly enhanced NO removal ratio of 50.7%, much higher than that of the pristine BiOI (1.2%). Density functional theory calculations and experimental results revealed that the Bi/BiOI/(BiO)2CO3 composites promoted the production of reactive oxygen species for photocatalytic NO oxidation. Thus, this work provides a new strategy to modify narrow-band semiconductors and explore other bismuth-containing heterostructured visible-light-driven photocatalysts.

Pivotal roles of artificial oxygen vacancies in enhancing photocatalytic activity and selectivity on Bi_2O_2CO_3 nanosheets

There is an increasing interest in bismuth carbonate(Bi2O2CO3,BOC)as a semiconductor photocatalyst.However,pure BOC strongly absorbs ultraviolet light,which drives a high recombination rate of charge carriers and thereby limits the overall photocatalysis efficiency.In this work,artificial oxygen vacancies(OV)were introduced into BOC(OV-BOC)to broaden the optical absorption range,increase the charge separation efficiency,and activate the reactants.The photocatalytic removal ratio of NO was increased significantly from 10.0%for pure BOC to 50.2%for OV-BOC because of the multiple roles played by the oxygen vacancies.These results imply that oxygen vacancies can facilitate the electron exchange between intermediates and the surface oxygen vacancies in OV-BOC,making them more easily destroyed by active radicals.In situ DRIFTS spectra in combination with electron spin resonance spectra and density functional theory calculations enabled unraveling of the conversion pathway for the photocatalytic NO oxidation on OV-BOC.It was found that oxygen vacancies could increase the production of active radicals and promote the transformation of NO into target products instead of toxic byproducts(NO2),thus the selectivity is significantly enhanced.This work provides a new strategy for enhancing photocatalytic activity and selectivity.