Liu Xiang, Han Xinglong, Liang Zhangqian, Xue Yanjun, Zhou Yanli, Zhang Xiaoli, Cui Hongzhi, Tian Jian
School of Materials Science and Engineering, Shandong University of Science and Technology, Qingdao 266590, China.
School of Environmental and Material Engineering, Yantai University, Yantai 264005, China.
J Colloid Interface Sci. 2022 Jan;605:320-329. doi: 10.1016/j.jcis.2021.07.111. Epub 2021 Jul 24.
Herein, we report that the phosphorous-doped 1 T-MoS as co-catalyst decorated nitrogen-doped g-CN nanosheets (P-1 T-MoS@N-g-CN) are prepared by the hydrothermal and annealing process. The obtained P-1 T-MoS@N-g-CN composite presents an enhanced photocatalytic N reduction rate of 689.76 μmol L gh in deionized water without sacrificial agent under simulated sunlight irradiation, which is higher than that of pure g-CN (265.62 μmol L gh), 1 T-MoS@g-CN (415.57 μmol L gh), 1 T-MoS@N doped g-CN (469.84 μmol L gh), and P doped 1 T-MoS@g-CN (531.24 μmol L gh). In addition, compared with pure g-CN NSs (2.64 mmol L gh), 1 T-MoS@g-CN (4.98 mmol L gh), 1 T-MoS@N doped g-CN (6.21 mmol L gh), and P doped 1 T-MoS@g-CN (9.78 mmol L gh), P-1 T-MoS@N-g-CN (11.12 mmol L gh) composite also shows a significant improvement for photocatalytic N fixation efficiency in the sacrificial agent (methanol). The improved photocatalytic activity of P-1 T-MoS@N-g-CN composite is ascribed to the following advantages: 1) Compared to pure g-CN, P-1 T-MoS@N-g-CN composite shows higher light absorption capacity, which can improve the utilization rate of the catalyst to light; 2) The P doping intercalation strategy can promote the conversion of 1 T phase MoS, which in turn in favor of photogenerated electron transfer and reduce the recombination rate of carriers; 3) A large number of active sites on the edge of 1 T-MoS and the existence of N doping in g-CN contribute to photocatalytic N fixation.
在此，我们报道了通过水热和退火工艺制备了磷掺杂的1T-MoS作为共催化剂修饰的氮掺杂g-CN纳米片（P-1T-MoS@N-g-CN）。在模拟太阳光照射下，所得的P-1T-MoS@N-g-CN复合材料在无牺牲剂的去离子水中呈现出增强的光催化固氮速率，为689.76 μmol L⁻¹ g⁻¹ h⁻¹，高于纯g-CN（265.62 μmol L⁻¹ g⁻¹ h⁻¹）、1T-MoS@g-CN（415.57 μmol L⁻¹ g⁻¹ h⁻¹）、1T-MoS@N掺杂g-CN（469.84 μmol L⁻¹ g⁻¹ h⁻¹）和P掺杂1T-MoS@g-CN（531.24 μmol L⁻¹ g⁻¹ h⁻¹）。此外，与纯g-CN纳米片（2.64 mmol L⁻¹ g⁻¹ h⁻¹）、1T-MoS@g-CN（4.98 mmol L⁻¹ g⁻¹ h⁻¹）、1T-MoS@N掺杂g-CN（6.21 mmol L⁻¹ g⁻¹ h⁻¹）和P掺杂1T-MoS@g-CN（9.78 mmol L⁻¹ g⁻¹ h⁻¹）相比，P-1T-MoS@N-g-CN（11.12 mmol L⁻¹ g⁻¹ h⁻¹）复合材料在牺牲剂（甲醇）中光催化固氮效率也有显著提高。P-1T-MoS@N-g-CN复合材料光催化活性的提高归因于以下优点：1）与纯g-CN相比，P-1T-MoS@N-g-CN复合材料表现出更高的光吸收能力，这可以提高催化剂对光的利用率；2）P掺杂插层策略可以促进1T相MoS的转化，进而有利于光生电子转移并降低载流子复合率；3）1T-MoS边缘的大量活性位点以及g-CN中N掺杂的存在有助于光催化固氮。
