Achievement of visible-light-driven Z-scheme overall water splitting using barium-modified Ta(3)N(5) as a H(2)-evolving photocatalyst.
Achievement of visible-light-driven Z-scheme overall water splitting using barium-modified Ta(3)N(5) as a H(2)-evolving photocatalyst.
复制标题
利用钡改性的Ta（3）N（5）作为释放H（2）的光催化剂实现可见光驱动的Z方案整体水裂解。
DOI：
10.1039/c6sc02750d
复制
发表时间：
2017-01-01
期刊：
影响因子：
8.4
通讯作者：
Li C
中科院分区：
文献类型：
--
作者：
Qi Y;Chen S;Li M;Ding Q;Li Z;Cui J;Dong B;Zhang F;Li C
钡改性的Ta 3 N5促进质子还原首次被用作可见光驱动的Z-方案整体水分解的H2-释放光催化剂。Ta 3 N5是用于太阳能水分解的最有前途的光催化剂候选者之一，但无论使用一步法还是两步法，通过Ta 3 N5基光催化剂实现整体水分解仍然具有挑战性。在这里，我们将解决相对较差的光催化质子还原Ta 3 N5的努力，促进通过钡改性的电荷分离。采用一锅氮化法对浸渍了硝酸锌的Ta_2O_5前驱体进行氮化，制备了Ta_3N_5/BaTaO_2N异质结构，并进行了表面钝化处理。由于改善的界面电荷分离和降低的缺陷密度的协同作用，钡改性Ta 3 N5的光催化析氢速率得到有效的促进。在此基础上，利用钡改性Ta 3 N5作为放氢光催化剂，PtOx/WO 3和IO 3-/I-分别作为放氧光催化剂和氧化还原介体，成功构建了可见光驱动的Z-模式整体水裂解体系。
Barium-modified Ta3N5 for the promotion of proton reduction is first employed as a H2-evolving photocatalyst for visible-light-driven Z-scheme overall water splitting. Ta3N5 is one of the most promising photocatalyst candidates for solar water splitting, but it still remains challenging to achieve overall water splitting via Ta3N5-based photocatalysts regardless of whether it uses a one step or two step method. Here we will address the relatively poor photocatalytic proton reduction of Ta3N5 with an effort for the promotion of charge separation via barium modification. One-pot nitridation of barium nitrate-impregnated Ta2O5 precursor was adopted here for the synthesis of Ta3N5 accompanied with the creation of a Ta3N5/BaTaO2N heterostructure and surface passivation. Due to the synergetic effect of the improved interfacial charge separation and the decreased defect density, the photocatalytic H2 evolution rate of barium-modified Ta3N5 is effectively promoted. Encouraged by this, a visible-light-driven Z-scheme overall water splitting system was successfully constructed by using the barium-modified Ta3N5 as a H2-evolving photocatalyst, together with a PtOx/WO3 and IO3 –/I– pair as an O2-evolving photocatalyst and a redox mediator, respectively.