可见光驱动改性氮化碳无牺牲剂光催化析氢

doi:10.1016/S1872-2067(21)64015-9

摘要/Abstract

摘要：

载铂石墨氮化碳(g-C₃N₄)是一种较好的可见光下催化析氢光催化剂. 但催化水裂解需要牺牲电子供体, 如三乙醇胺等. 目前, 无牺牲剂条件下g-C₃N₄的催化析氢仍是一个挑战. 本文通过尿素热处理制备了氮化碳纳米片(NS-C₃N₄), 并研究了其在可见光(λ > 400 nm)下利用可逆电子给体无牺牲剂条件下析氢的光催化活性. 在含有I^-, Fe²⁺或[Fe(CN)₆]^4-的水溶液中, 负载铂的NS-C₃N₄上无H₂产生, 用CrO_x改性Pt/NS-C₃N₄的光催化剂上可观察到H₂的析出. 透射电镜和能量色散X射线光谱结果表明, 在NS-C₃N₄上形成了Pt/CrO_x核壳结构. 在[Fe(CN)₆]^3-/4-氧化还原介质存在下, CrO_x/Pt/NS-C₃N₄与改性WO₃光催化剂在可见光下共同催化水分解析氢.

关键词: 人工光合成, 太阳燃料, 水分解

Abstract:

Pt-loaded graphitic carbon nitride (g-C₃N₄) is known to be a good photocatalyst for H₂ evolution under visible light. In most cases, however, sacrificial electron donors such as triethanolamine are required for the water-splitting operation, and nonsacrificial H₂ evolution by g-C₃N₄ remains a challenge. In this work, we investigated the photocatalytic activities of carbon nitride nanosheet (NS-C₃N₄), which was prepared by thermal treatment of urea, for nonsacrificial H₂ evolution using reversible electron donors under visible light (λ > 400 nm). Whereas Pt-loaded NS-C₃N₄ did not produce H₂ from aqueous solutions containing I^-, Fe²⁺, or [Fe(CN)₆]^4-, modification of the Pt/NS-C₃N₄ photocatalyst with CrO_x led to observable H₂ evolution. Transmission electron microscopy observations and energy-dispersive X-ray spectroscopic analysis suggested that a Pt-core/CrO_x-shell structure was formed on the NS-C₃N₄. The CrO_x/Pt/NS-C₃N₄ served as a H₂-evolution photocatalyst for visible-light-driven Z-scheme overall water splitting, in combination with a modified WO₃ photocatalyst, in the presence of a [Fe(CN)₆]^3-/4- redox mediator.

Key words: Artificial photosynthesis, Solar fuels, Water splitting

Shunta Nishioka, Kengo Shibata, Yugo Miseki, Kazuhiro Sayama, Kazuhiko Maeda. 可见光驱动改性氮化碳无牺牲剂光催化析氢[J]. 催化学报, 2022, 43(9): 2316-2320.

Shunta Nishioka, Kengo Shibata, Yugo Miseki, Kazuhiro Sayama, Kazuhiko Maeda. Visible-light-driven nonsacrificial hydrogen evolution by modified carbon nitride photocatalysts[J]. Chinese Journal of Catalysis, 2022, 43(9): 2316-2320.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(21)64015-9

https://www.cjcatal.com/CN/Y2022/V43/I9/2316

图/表 5

Fig. 1. TEM images of NS-C3N4 with various modifications. The inset images in the left and center panels show the corresponding high-resolution or magnified views. The initial loading amounts of Pt and Cr were 1.0 wt% and 3 wt%, respectively.

Fig. 2. STEM-EDS mapping images of CrOx/Pt/NS-C3N4. The initial loading amounts of Pt and Cr were 1 wt% and 3 wt%, respectively. (a) STEM images. (b?d) Signals of carbon, platinum and chromium species from the CrOx/Pt/NS-C3N4, respectively.

Table 1 Photocatalytic activities of NS-C3N4 with and without the Pt or the CrOx modification for H2 evolution from aqueous solutions containing various electron donors under visible light (λ > 400 nm).

Entry	Cocatalyst	Electron donor	pH	Amount of evolved H₂ for 5 h (μmol)
1	Pt	Methanol	—	17.4
2	Pt	KI	5.6	n.d.
3	Pt	FeCl₂	3.0	n.d.
4	Pt	K₄[Fe(CN)₆]	7.1	n.d.
5	CrO_x/Pt	Methanol	—	22.3
6	CrO_x/Pt	KI	5.9	0.9
7	CrO_x/Pt	FeCl₂	3.0	1.5
8	CrO_x/Pt	K₄[Fe(CN)₆]	7.2	1.1
9	CrO_x	Methanol	—	n.d.
10	CrO_x	K₄[Fe(CN)₆]	7.2	n.d.

Fig. 3. Time courses of H2 evolution from aqueous K4[Fe(CN)6] solution (1 mmol/L) using CrOx/Pt/NS-C3N4 with and without the intentional addition of K3[Fe(CN)6] (0.1 mmol/L); the reaction was conducted under visible light (λ > 400 nm). Reaction conditions: catalyst, 25 mg; reactant solution, aqueous solution (140 mL); light source, Xe lamp (300 W) with a cold mirror (CM-1) and a cutoff filter (L42).

Fig. 4. Time course of H2 and O2 evolution from a mixture of CrOx/Pt/NS-C3N4 (2.5 mg) and Fe-H-Cs-WO3 (50 mg) dispersed in an aqueous K4[Fe(CN)6] solution (140 mL, 0.5 mmol/L); the reaction was conducted under visible-light irradiation.

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