新型PtPd合金纳米颗粒修饰g-C3N4纳米片以提高可见光照射下光催化产氢活性

doi:10.1016/S1872-2067(18)63180-8

催化学报 ›› 2019, Vol. 40 ›› Issue (3): 352-361.DOI: 10.1016/S1872-2067(18)63180-8

新型PtPd合金纳米颗粒修饰g-C₃N₄纳米片以提高可见光照射下光催化产氢活性

肖楠^a,b, 李松松^b, 刘霜^b, 徐博冉^b, 李延东^b, 高旸钦^b, 戈磊^a,b, 卢贵武^b

a 中国石油大学(北京)重质油国家重点实验室, 北京 102249;
b 中国石油大学(北京)新能源与材料学院, 北京 102249

收稿日期:2018-08-06 修回日期:2018-09-25 出版日期:2019-03-18 发布日期:2019-02-22
通讯作者: 戈磊
基金资助:
国家自然科学基金（51572295，21273285，21003157）；北京新星计划（2008B76）；中国石油大学（北京）科学基金（KYJJ2012-06-20，2462016YXBS05）.

Novel PtPd alloy nanoparticle-decorated g-C₃N₄ nanosheets with enhanced photocatalytic activity for H₂ evolution under visible light irradiation

Nan Xiao^a,b, Songsong Li^b, Shuang Liu^b, Boran Xu^b, Yandong Li^b, Yangqin Gao^b, Lei Ge^a,b, Guiwu Lu^b

a State Key Laboratory of Heavy Oil Processing, China University of Petroleum Beijing, Beijing 102249, China;
b College of New Energy and Materials, China University of Petroleum Beijing, Beijing 102249, China

Received:2018-08-06 Revised:2018-09-25 Online:2019-03-18 Published:2019-02-22
Supported by:
This work was supported by the National Natural Science Foundation of China (51572295, 21273285, 21003157), the Beijing Nova Program (2008B76), and the Science Foundation of China University of Petroleum Beijing (KYJJ2012-06-20 and 2462016YXBS05).

摘要/Abstract

摘要：

石墨相氮化碳（g-C₃N₄）纳米片因其廉价、易得、无毒等优点而在光催化领域被广泛应用和研究.但单一的g-C₃N₄存在光生电子与空穴易复合等缺陷，而助催化剂的存在可以促进电荷转移，延长载流子寿命，从而提高光催化性能.本文通过合成PtPd双金属合金纳米颗粒作为助催化剂，对g-C₃N₄纳米片光催化剂进行修饰以提高可见光照射下的光催化产氢速率.
g-C₃N₄是以尿素为原材料，通过高温热缩聚和热刻蚀的方法合成，PtPd/g-C₃N₄复合光催化剂通过化学还原沉积法合成.对所获得的复合光催化剂进行了XRD测试并将结果与PdPt标准卡片进行了对比，结果表明，各峰的位置都能有较好的对应，说明成功合成了PdPt.采用TEM对PtPd/g-C₃N₄的形貌进行观察，发现g-C₃N₄呈薄片状，且PdPt颗粒较为均匀地分布在其表面.XPS测试发现，PtPd/g-C₃N₄复合样品中Pt和Pd元素的峰值较Pt/g-C₃N₄和Pd/g-C₃N₄均发生0.83 eV的偏移，进一步说明合成了PtPd双金属合金纳米颗粒.DRS测试表明，g-C₃N₄的带隙宽度为2.69 eV，而PtPd双金属合金纳米颗粒的负载有效地减小了禁带宽度，从而提高了光催化剂对光的利用率.
光催化产氢性能实验发现，当g-C₃N₄负载PtPd双金属合金纳米颗粒后，光催化产氢速率大幅度提高，其中负载量为0.2 wt%的PtPd/g-C₃N₄复合光催化剂的产氢速率最高，为1600.8 μmol g^-1 h^-1，是纯g-C₃N₄纳米片的800倍.向光催化体系中添加10 g K₂HPO₄后，产氢速率提高到2885.0 μmol g^-1 h^-1.当二元合金中Pt：Pd比为1：1时，PtPd/g-C₃N₄复合光催化剂上的产氢速率最高，分别是Pt/g-C₃N₄和Pd/g-C₃N₄上的3.6倍和1.5倍.另外，在420 nm处量子效率为5.5%.PtPd/g-C₃N₄复合光催化剂还表现出很好的稳定性，能够在完成4次光催化实验循环后仍然保持其良好的光催化活性.
对PtPd/g-C₃N₄复合光催化剂进行了一系列光电化学表征.PL结果表明，PtPd/g-C₃N₄复合光催化剂与纯g-C₃N₄相比荧光强度减弱，说明PtPd/g-C₃N₄复合光催化剂有较慢的光生电子-空穴复合速率，这可以更有效地使电荷分离，从而提高光催化活性.根据光催化反应和表征分析结果提出了复合光催化剂上水分解产氢可能的机理，即PtPd/g-C₃N₄之间的协同作用有助于提高复合光催化剂的光催化活性.

关键词: g-C₃N₄纳米片, PtPd合金纳米颗粒, 产氢, 光催化

Abstract:

PtPd bimetallic alloy nanoparticle (NP)-modified graphitic carbon nitride (g-C₃N₄) nanosheet photocatalysts were synthesized via chemical deposition precipitation. Characterization of the photocatalytic H₂ evolution of the g-C₃N₄ nanosheets shows that it was significantly enhanced when PtPd alloy NPs were introduced as a co-catalyst. The 0.2 wt% PtPd/g-C₃N₄ composite photocatalyst gave a maximum H₂ production rate of 1600.8 μmol g^-1 h^-1. Furthermore, when K₂HPO₄ was added to the reaction system, the H₂ production rate increased to 2885.0 μmol g^-1 h^-1. The PtPd/g-C₃N₄ photocatalyst showed satisfactory photocatalytic stability and was able to maintain most of its photocatalytic activity after four experimental photocatalytic cycles. In addition, a possible mechanism for the enhanced photocatalytic activity was proposed and verified by various photoelectric techniques. These results demonstrate that the synergistic effect between PtPd and g-C₃N₄ helps to greatly improve the photocatalytic activity of the composite photocatalyst.

Key words: g-C₃N₄ nanosheets, PtPd alloy nanoparticles, H₂ evolution, Photocatalysis

肖楠, 李松松, 刘霜, 徐博冉, 李延东, 高旸钦, 戈磊, 卢贵武. 新型PtPd合金纳米颗粒修饰g-C₃N₄纳米片以提高可见光照射下光催化产氢活性[J]. 催化学报, 2019, 40(3): 352-361.

Nan Xiao, Songsong Li, Shuang Liu, Boran Xu, Yandong Li, Yangqin Gao, Lei Ge, Guiwu Lu. Novel PtPd alloy nanoparticle-decorated g-C₃N₄ nanosheets with enhanced photocatalytic activity for H₂ evolution under visible light irradiation[J]. Chinese Journal of Catalysis, 2019, 40(3): 352-361.

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新型PtPd合金纳米颗粒修饰g-C₃N₄纳米片以提高可见光照射下光催化产氢活性

Novel PtPd alloy nanoparticle-decorated g-C₃N₄ nanosheets with enhanced photocatalytic activity for H₂ evolution under visible light irradiation

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