当前位置：
X-MOL 学术
›
J. Phys. Chem. C
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Insight into the Effect of the Cl 3p Orbital on g-C3N4 Mimicking Photosynthesis under CO2 Reduction
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-04-28 , DOI: 10.1021/acs.jpcc.1c00663 Yi Wang 1 , Xu Tang 2 , Pengwei Huo 2 , Yongsheng Yan 2 , Zhi Zhu 2 , Jiangdong Dai 2 , Zhixiang Liu 3 , Zhanguo Li 1 , Hailing Xi 1
The Journal of Physical Chemistry C ( IF 3.3 ) Pub Date : 2021-04-28 , DOI: 10.1021/acs.jpcc.1c00663 Yi Wang 1 , Xu Tang 2 , Pengwei Huo 2 , Yongsheng Yan 2 , Zhi Zhu 2 , Jiangdong Dai 2 , Zhixiang Liu 3 , Zhanguo Li 1 , Hailing Xi 1
Affiliation
|
Achieving high-efficiency photocatalytic materials to convert CO2 into high-value chemicals is still challenging. Herein, chlorine-doped g-C3N4 photocatalysts (Cl-CN) were successfully synthesized by a simple multiple calcination method. The as-prepared Cl-CN exhibited satisfactory photocatalytic activity in photoreduction of CO2. The CO yield of Cl-CN was about 39.89 μmol/g. The DRS, UPS, and VB-XPS results indicated a narrower band gap, and the negatively shifted CB potential enhanced the CO2 reduction ability. DFT calculations and the partial density of states revealed that the Cl 3p orbital greatly contributed to the CBM and VBM of Cl-CN, which caused the narrower band gap and an upshift of the conduction band by 0.14 eV over that of bulk-CN. The CO2 conversion intermediate was investigated by in situ Fourier transform infrared spectroscopy, and the corresponding reaction mechanism was proposed according to the density functional theory calculations and experimental results, which showed that Cl doping and the C–Cl bond increased the photogenerated carrier lifetime and the CO2 adsorption capacity of Cl-CN. Therefore, this work provides a deeper understanding of the effect of Cl doping on the g-C3N4 electronic structure and its CO2 reduction activity.
中文翻译：
在CO 2还原下Cl 3p轨道对模拟光合作用的gC 3 N 4的影响的见解
实现高效的光催化材料以将CO 2转化为高价值的化学物质仍然具有挑战性。本文中，通过简单的多重煅烧方法成功地合成了掺氯的gC 3 N 4光催化剂（Cl-CN）。所制备的Cl-CN在CO 2的光还原中表现出令人满意的光催化活性。Cl-CN的CO产率为约39.89μmol/ g。DRS，UPS和VB-XPS结果表明带隙较窄，并且CB电位负移增强了CO 2还原能力。DFT计算和状态的部分密度表明，Cl 3p轨道极大地促进了Cl-CN的CBM和VBM，这导致了较窄的CN窄的带隙和导带上移0.14 eV。通过原位傅里叶变换红外光谱研究了CO 2转化中间体，并根据密度泛函理论计算和实验结果提出了相应的反应机理，表明Cl掺杂和C–Cl键增加了光生载流子的寿命和Cl-CN的CO 2吸附能力。因此，这项工作使人们更深入地了解了Cl掺杂对gC 3 N 4的影响。电子结构及其CO 2还原活性
更新日期：2021-05-13
中文翻译：
在CO 2还原下Cl 3p轨道对模拟光合作用的gC 3 N 4的影响的见解
实现高效的光催化材料以将CO 2转化为高价值的化学物质仍然具有挑战性。本文中，通过简单的多重煅烧方法成功地合成了掺氯的gC 3 N 4光催化剂（Cl-CN）。所制备的Cl-CN在CO 2的光还原中表现出令人满意的光催化活性。Cl-CN的CO产率为约39.89μmol/ g。DRS，UPS和VB-XPS结果表明带隙较窄，并且CB电位负移增强了CO 2还原能力。DFT计算和状态的部分密度表明，Cl 3p轨道极大地促进了Cl-CN的CBM和VBM，这导致了较窄的CN窄的带隙和导带上移0.14 eV。通过原位傅里叶变换红外光谱研究了CO 2转化中间体，并根据密度泛函理论计算和实验结果提出了相应的反应机理，表明Cl掺杂和C–Cl键增加了光生载流子的寿命和Cl-CN的CO 2吸附能力。因此，这项工作使人们更深入地了解了Cl掺杂对gC 3 N 4的影响。电子结构及其CO 2还原活性
京公网安备 11010802027423号