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Potassium-Doped g-C3N4 Achieving Efficient Visible-Light-Driven CO2 Reduction
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2020-05-13 , DOI: 10.1021/acssuschemeng.0c01151
Shuhui Wang 1 , Jiawei Zhan 1 , Kui Chen 1 , Asad Ali 2 , Linghui Zeng 1 , He Zhao 1 , Wanglai Hu 3 , Lixin Zhu 2 , Xiaoliang Xu 1
Affiliation  

The visible-light-driven CO2 reduction efficiency is largely restrained by the negative photoabsorption and high recombination rate of electron–hole pairs. It is an effective method to increase the efficiency of CO2 photoreduction by doping alkali metal elements to engineer the electronic properties of the catalyst. Here, we report a new study on the potassium-doped g-C3N4 (K-CN) being used for CO2 reduction irradiated by visible light. DFT calculations and XPS tests show that the potassium doping is interlayer doping, changing the electronic structure of g-C3N4. The higher ID/IG value indicates more structural distortion and defects caused by K doping. K-CNs have enhanced visible-light absorption, and PL spectra demonstrate that the introduction of potassium advances the separation and transmission of photoexcited charge carriers, further confirmed by transient photocurrent response experiment. Under visible light, K-CN-7 achieved efficient CO2 reduction without any noble metal as a cocatalyst, with CO formation rates of 8.7 μmol g–1 h–1, which is 25 times that of ordinary g-C3N4. Our work further validates the importance of inhibiting e/h+ recombination in improving solar energy conversion efficiency while also bringing hope for efficient solar fuel production using g-C3N4.

中文翻译:

掺杂钾的gC 3 N 4可实现有效的可见光驱动的CO 2还原

负光吸收和电子-空穴对的高复合率在很大程度上限制了可见光驱动的CO 2还原效率。通过掺杂碱金属元素来控制催化剂的电子性能,是提高CO 2光还原效率的有效方法。在这里,我们报道了一项新的研究,即钾掺杂的gC 3 N 4(K-CN)被用于可见光照射下的CO 2还原。DFT计算和XPS测试表明,钾掺杂是层间掺杂,改变了gC 3 N 4的电子结构。I D / I G越高值表示由K掺杂引起的更多的结构变形和缺陷。K-CNs增强了可见光吸收,PL光谱表明钾的引入促进了光激发电荷载流子的分离和传输,这通过瞬态光电流响应实验进一步证实。在可见光下,K-CN-7在没有任何贵金属作为助催化剂的情况下实现了有效的CO 2还原,CO形成速率为8.7μmolg –1 h –1,是普通gC 3 N 4的25倍。我们的工作进一步证实了抑制e / h +的重要性。在提高太阳能转换效率的同时进行重组,也为使用gC 3 N 4高效生产太阳能带来希望。
更新日期:2020-05-13
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