内电场增强S型异质结N-C3N4/BiOClxI1−x的制备及其光催化性能

Preparation of S-type heterojunction N-C3N4/BiOClxI1−x with internal electric field and enhanced photocatalytic properties

  • 摘要: 采用一步水热法使固溶体BiOClxI1−x静电自组装在N掺杂的氮化碳(N-C3N4)表面,制备了N-C3N4/BiOClxI1−x S型异质结。通过XRD、XPS、SEM、TEM、FTIR、UV-Vis等技术对样品的晶型、形貌、结构、元素组成、表面官能团、光学性质等进行了表征,并考察了N-C3N4/BiOClxI1−x光催化氧化有机污染物与还原Cr(VI)的活性。结果表明,N-C3N4/BiOClxI1−x具有强的光吸收,在N-C3N4与BiOClxI1−x界面处形成的内电场抑制了电子-空穴对的复合。在可见光照射下,20%N-BiOCl0.5I0.5呈现出优异的光催化活性,2.5 h内苯酚的降解率达到98.53%;1 h内Cr(VI)的还原率达到99.11%。20%N-BiOCl0.5I0.5在5次循环后表现出良好的稳定性。3 h内20%N-BiOCl0.5I0.5可见光降解苯酚的总有机碳(TOC)去除率为80.21%。结合捕获实验、ESR、DFT计算等表明,N-C3N4/BiOClxI1−x活性归因于S型异质结的形成、N-C3N4和BiOClxI1−x之间的内部电场及能带弯曲和库仑力的存在,加速了光生载流子的空间分离和有序电子流。

     

    Abstract: N doped carbon nitride (N-C3N4)/BiOClxI1−x S-type heterojunctions were prepared by a facile one-step hydrothermal method. The crystal form, morphology, structure, elemental composition, surface functional groups and optical properties of the samples were characterized by XRD, XPS, SEM, TEM, FTIR and UV-Vis. The photocatalytic activity of N-C3N4/BiOClxI1−x oxidation of organic pollutants and reduction of Cr(VI) was investigated. The results show that N-C3N4/BiOClxI1−x sample exhibits the effective enhancement in light absorption. The charge carriers were generated by the transfer of the photoinduced electron from N-C3N4 to BiOClxI1−x across the interface under irradiation, which inhibited the recombination of electron-hole pairs. Under visible light irradiation, 20%N-BiOCl0.5I0.5 exhibited high activity, the degradation rate of phenol reached 98.53% with 2.5 h of visible light irradiation. Meanwhile, the reduction rate of Cr(VI) of 20%N-BiOCl0.5I0.5 reached to 99.11% with 1 h of visible light irradiation. 20%N-BiOCl0.5I0.5 showed good stability after five cycles. The total organic carbon (TOC) removal rate of degradation phenol by 20%N-BiOCl0.5I0.5 within 3 h was 80.21%. Combined with capture experiment, ESR and DFT calculation, the improvement activity of N-C3N4/BiOClxI1−x was attributed to the formation of S-type heterojunction, the internal electric field based on different Fermi levels between N-C3N4 and BiOClxI1−x, as well as band bending and Coulomb force, which together accelerated spatial separation of photogenerated carriers and orderly electron flow.

     

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