g-C<sub>3</sub>N<sub>4</sub>材料在光催化能源轉換領域的新進展

趙夢迪; 李永利; 王金淑

doi:10.13374/j.issn2095-9389.2021.09.01.001

g-C₃N₄材料在光催化能源轉換領域的新進展

doi: 10.13374/j.issn2095-9389.2021.09.01.001

北京工業大學材料與制造學部新型功能材料教育部重點實驗室，北京 100124

基金項目: 國家自然科學基金資助項目（51974011）；國家創新群體資助項目（51621003）；北京長城學者研究計劃資助項目（20190307）

詳細信息

通訊作者:
李永利，E-mail: lyl@bjut.edu.cn

王金淑，E-mail: wangjsh@bjut.edu.cn

中圖分類號: TG142.71
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- 被引次數: 0
出版歷程
- 收稿日期: 2021-09-01
- 網絡出版日期: 2021-10-19
- 刊出日期: 2022-04-02

Recent progress of graphitic phase carbon nitride photocatalytic materials on solar energy conversion

Key Laboratory of Advanced Functional Materials, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing 100124, China

More Information

Corresponding author: LI Yong-li, E-mail: lyl@bjut.edu.cn; WANG Jin-shu, E-mail: wangjsh@bjut.edu.cn

摘要

摘要: 類石墨相氮化碳（g-C₃N₄）作為當前光催化領域的熱點材料，盡管在可見光響應范圍和載流子的遷移/分離方面不如人意，但其不含金屬、穩定性好，結構易于調控等優點依然備受關注，尤其是近年來基于g-C₃N₄的形貌與電子結構調控取得了大量的突破性進展。本文系統地綜述了針對g-C₃N₄缺陷的不同改性和優化方法，從形貌調控、結構優化、構建異質結三方面介紹了g-C₃N₄光催化材料的最新研究進展，重點闡述了針對改善光催化分解水效率的各種改性優化策略。以材料的維度尺寸作為切入點介紹了不同形貌g-C₃N₄的制備方法，從摻雜與缺陷調控角度總結了g-C₃N₄結構與光生載流子分離以及催化性能的關系，并且依據不同異質結類型歸納了g-C₃N₄基光催化材料體系。最后，對g-C₃N₄基光催化材料今后的發展與面臨的挑戰進行了展望和總結。
- 類石墨相氮化碳(g-C₃N₄) /
- 形貌調控 /
- 結構優化 /
- 異質結構建 /
- 光催化析氫
Abstract: With the increasing consumption of fossil fuels, severe energy shortages and environmental issues are fast approaching. Therefore, the development of green energy resources is urgently appealed. Among them, the sunlight-driven production of hydrogen fuel with suitable photocatalysts is regarded as one of the potential strategies to meet the sustainable energy demand in the future. However, photocatalysis still faces significant uncertainties mainly because of the notorious photogenerated electron-hole (e-h) recombination and low carriers’ mobility. To achieve high photocatalytic performance, it is essential to tailor the spatial charge separation and fast charge transfer via electronic and structural manipulation of photocatalysts. As one of the hot-spot photocatalysts, graphitic phase carbon nitride (g-C₃N₄) has received tremendous attention in the study of solar-to-fuel (STF) conversion and carbon dioxide reduction reactions (CO₂RR), owing to intrinsic merits, such as metal-free components, low-cost resources, good stability, and visible light response. Recently, considerable progress has been achieved to improve the photocatalytic STF efficiency of g-C₃N₄-based materials by developing strategies of structures and electric configurations engineering. In this study, different modification methods for g-C₃N₄ were systematically reviewed from the perspective of defects control to provide a new understanding of its structure-function relationship. Particularly, this study was composed in detail from three aspects to demonstrate the latest research progress of g-C₃N₄ photocatalytic materials. First, different routes toward g-C₃N₄ with different shapes were introduced, including 1D, 2D, and 3D. Second, doping effects and defect control on the separation and transfer of photogenerated electron-hole pairs were carefully reviewed. Finally, heterojunctions based on g-C₃N₄ were summarized, highlighting the Z-scheme heterojunction. In addition, some future directions and challenges for the enhancement of the photocatalytic efficiency upon g-C₃N₄ were pointed out according to our understanding of photocatalytic water splitting.
- graphitic phase carbon nitride (g-C₃N₄) /
- morphological control /
- structural engineering /
- heterojunction construction /
- photocatalytic hydrogen evolution

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圖 1 0D/2D g-CNQDs/PMOF光催化還原二氧化碳生成CH₄過程示意圖^[35]

Figure 1. Schematic of the 0D/2D g-CNQDs/PMOF photocatalytic reduction of carbon dioxide to CH₄^[35]

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圖 2 g-C₃N₄納米管的形成過程^[41]

Figure 2. Formation process of graphitic phase carbon nitride nanotubes^[41]

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圖 3 （a）二維氮化碳（550 ℃, 2 h）的掃描電鏡形貌；（b~g）在不同保溫時間下（0, 0.5, 1, 1.5, 2, 2.5 h）550 ℃熱處理制得g-C₃N₄的掃描電鏡形貌；（h~i）550 ℃保溫1.5 h后制得g-C₃N₄的掃描電鏡和透射電鏡形貌^[53]

Figure 3. (a) Scanning electron microscopy (SEM) images of two-dimensional carbon nitride (550 ℃, 2 h); （b?g） SEM images of the g-C₃N₄ from layered organic materials in different heat preservation time at 550 ℃ with holding times of 0 h, 0.5 h, 1 h, 1.5 h, 2 h, and 2.5 h; (h–i) SEM and transmission electron microscopy images of graphitic phase carbon nitride prepared by CN at 550 ℃ for 1.5 h^[53]

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圖 4 （a）爐內空氣冷卻的g-C₃N₄ (ACN)和三維分級多孔g-C₃N₄（HCN）的實驗過程示意圖；（b,c）HCN的場發射掃描電鏡圖像；（d）HCN的透射電鏡圖像^[56]

Figure 4. (a) Schematic of the experimental process of ACN and HCN; (b,c) FESEM image of HCN; (d) transmission electron microscopy image of HCN^[56]

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圖 5 （a）分層C₃N₄納米結構的氣固生長示意圖；（b）薄膜上C₃N₄納米結構的光學顯微像(OM)；（c,d）薄膜上C₃N₄納米結構的掃描電鏡照片^[60]

Figure 5. (a) Gas–solid growth diagram of layered C₃N₄ nanostructures; (b) optical microscope images of C₃N₄ nanostructures on thin films; (c and d) scanning electron microscopy images of C₃N₄ nanostructures on thin films^[60]

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圖 6 P-g-C₃N₄的形成過程^[67]

Figure 6. Formation process of P-g-C₃N₄^[67]

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圖 7 p區元素摻雜的g-C₃N₄電子結構.（a）摻雜能級為1.69 eV的N摻雜g-C₃N₄能帶結構（左）和相應的態密度（右）；（b）不同摻雜劑摻雜的g-C₃N₄直接帶隙；（c）各種元素摻雜g-C₃N₄的導帶（CB，黑色）和價帶（VB，紅色）邊緣位置^[72]

Figure 7. Electronic structure of the p-block element doped graphitic phase carbon nitride (g-C₃N₄): (a) band structure of N-doped g-C₃N₄ with a doping energy level of 1.69 eV (left) and the corresponding partial state density (right); (b) direct band gap of g-C₃N₄ doped with different dopants; (c) conduction band (black) and valence band (VB, red) edge positions of doped g-C₃N₄^[72]

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圖 8 基于EDA氣?固反應的g-C₃N₄不對稱結構調控設計及合成路線^[74]

Figure 8. Conceptual design and synthetic route for the asymmetric structure engineering of melon-based graphitic phase carbon nitride through the EDA-induced gas–solid reaction^[74]

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圖 9 在不同氣氛下對g-C₃N₄進行連續熱處理制備富碳g-C₃N₄納米片的過程示意圖^[79]

Figure 9. Preparation of carbon-rich graphitic phase carbon nitride (g-C₃N₄) nanosheets by continuous heat treatment of g-C₃N₄ in different atmospheres^[79]

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圖 10 不同類型的g-C₃N₄基異質結系統的電荷轉移機制^[81]

Figure 10. Charge-transfer mechanisms in different types of g-C₃N₄-based heterojunction systems^[81]

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圖 11 催化劑的合成及微觀形貌。（a）由CNN衍生的BDCNN合成原理圖；（b,c）CNN和BDCNN的透射電鏡照片；（d,e）CNN和BDCNN在硅片上的原子力顯微鏡圖像及高度輪廓線^[95]

Figure 11. Catalyst synthesis and microscopy: (a) schematic of the synthesis of BDCNN derived from CNN; transmission electron microscopy images of CNN (b) and BDCNN (c); AFM images of CNN (d) and BDCNN (e) on a silicon wafer with the height profile determined along the lines shown in the insets^[95]

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