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Green synthesis of boron and nitrogen co-doped TiO2 with rich B-N motifs as Lewis acid-base couples for the effective artificial CO2 photoreduction under simulated sunlight
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2020-11-25 , DOI: 10.1016/j.jcis.2020.11.075
Dapeng Wu , Jing Guo , Hongju Wang , Xilin Zhang , Yonggang Yang , Can Yang , Zhiyong Gao , Zichun Wang , Kai Jiang

Boron and nitrogen co-doped Titanium dioxide (TiO2) nanosheets (BNT) with high surface area of 136.5 m2 g−1 were synthesized using ammonia borane as the green and triple-functional regent, which avoids the harmful and explosive reducing regents commonly used to create surface defects on TiO2. The decomposition of ammonia borane could incorporate reactive Lewis acid-base (B, N) pairs, together with the as-generated H2 to create mesoporous structure and rich oxygen vacancies in pristine TiO2. The BNTs prepared from various ammonia borane loading are evaluated in photoreduction of carbon dioxide (CO2) with steam under simulated sunlight, achieving about 3.5 times higher carbon monoxide (CO) production than pristine TiO2 under the same conditions. Steady state and transient optical measurements indicated BNT with reduced band gap, rich defect states and elevated conduction band position could enhance the light harvesting efficiency and promote the charge transfer at the catalyst/CO2 interface. Density functional theory simulation and in situ FTIR suggest that the Lewis acid-base (B, N) pairs on BNT may very substantially increase the activation of inert CO2 which facilitates their photoreduction with the hydrogen from the water splitting at the surface defects on TiO2. Finally, a reaction mechanism of Lewis acid-base assisted CO2 photoreduction leading to substantially improved performance is proposed.



中文翻译:

在模拟阳光下绿色合成有效合成CO 2的硼和氮共掺杂的TiO 2和富BN图案的路易斯酸-碱对偶合剂。

以氨硼烷为绿色和三功能试剂,合成了高表面积136.5 m 2 g -1的硼氮共掺杂二氧化钛(TiO 2)纳米片(BNT),避免了有害和爆炸性还原剂的普遍使用。用于在TiO 2上产生表面缺陷。氨硼烷的分解可以结合反应性路易斯酸碱(B,N)对,以及生成的H 2,在原始TiO 2中产生介孔结构和富氧空位。在二氧化碳(CO 2)的光还原中,评估了由各种氨硼烷负载量制备的BNT)在模拟阳光下使用蒸汽,在相同条件下,其一氧化碳(CO)产量比原始TiO 2高约3.5倍。稳态和瞬态光学测量表明,BNT的带隙减小,缺陷状态丰富和导带位置升高,可以提高光收集效率并促进催化剂/ CO 2界面上的电荷转移。密度泛函理论模拟和原位FTIR表明,BNT上的路易斯酸碱(B,N)对可能极大地增加了惰性CO 2的活化,从而促进了其的光还原,其中水被氢分解为TiO上的表面缺陷而使氢发生光还原。2。最后,提出了路易斯酸碱辅助的CO 2光还原反应导致性能显着提高的反应机理。

更新日期:2020-12-03
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