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中文題目：3D多孔g-C₃N₄/GO骨架穩(wěn)定貴金屬助催化劑增強(qiáng)日光誘導(dǎo)產(chǎn)氫活性

Title: Enhanced cocatalyst-support interaction and promoted electron transfer of 3D porous g-C₃N₄/GO-M (Au, Pd, Pt) composite catalysts for hydrogen evolution

作者：李偉* 褚曉姍 王菲 黨妍妍 劉小云 王學(xué)川* 王傳義*

關(guān)鍵字：Simulated solar light; Hydrogen evolution reaction; Precious metal; Three-dimensional porous structure; Electron acceptor

論文來源：期刊論文

具體來源：https://doi.org/10.1016/j.apcatb.2021.120034

發(fā)表時(shí)間：2021年

研究背景：

隨著經(jīng)濟(jì)的快速發(fā)展及人類生活需求的不斷增長，環(huán)境與能源問題日益凸顯。解決環(huán)境污染和能源短缺問題已迫在眉睫。氫能源是一種綠色、可持續(xù)新能源，通過光催化技術(shù)有效產(chǎn)氫是目前能源材料領(lǐng)域研究的熱點(diǎn)。

研究內(nèi)容：

鑒于石墨烯及碳氮化合物（g-C₃N₄）表現(xiàn)出的諸多優(yōu)越性能在光催化劑合成中具有重要應(yīng)用。本研究通過模板輔助法構(gòu)筑3D多孔g-C₃N₄/GO (p-CNG)復(fù)合骨架。基于3D p-CNG復(fù)合骨架適宜的孔徑尺寸及結(jié)構(gòu)中大量官能團(tuán)的配位效應(yīng)，可以將貴金屬(Au、Pd、Pt)助催化劑穩(wěn)定固定在3D p-CNG復(fù)合骨架結(jié)構(gòu)中，構(gòu)筑出3D p-CNG-M (Au、Pd、Pt)復(fù)合催化劑。作為電子受體的貴金屬助催化劑顯著增加了復(fù)合結(jié)構(gòu)的催化活性位點(diǎn)，促進(jìn)了電子-空穴分離，從而在模擬日光(SSL)誘導(dǎo)下表現(xiàn)出顯著增強(qiáng)的催化產(chǎn)氫活性。研究表明，當(dāng)pH = 10.5時(shí)，助催化劑-載體相互作用最強(qiáng)，是的優(yōu)化后的3D p-CNG-Pt復(fù)合催化劑產(chǎn)氫活性更為突出(2565.81 μmol·g^-1·h^-1)，其活性可以達(dá)到3D p-CNG復(fù)合骨架(18.93 μmol·g^-1·h^-1)的136倍。在λ = 420 nm的誘導(dǎo)光下，其表觀量子產(chǎn)率達(dá)到了21.6%。鑒于優(yōu)化催化劑穩(wěn)定的架構(gòu)優(yōu)勢，其在長時(shí)間的光誘導(dǎo)和多次循環(huán)利用過程中均表現(xiàn)出優(yōu)異的催化持久性和重復(fù)使用性。

Fig.1 Synthetic diagram of 3D p-CNG-M (Au, Pd, Pt) composite catalysts.

研究意義：

本研究為增強(qiáng)貴金屬修飾光催化劑的結(jié)構(gòu)穩(wěn)定性并提高其催化產(chǎn)氫性能提供了一種有效策略。

部分表征及性能數(shù)據(jù)如下圖所示：

Fig.2 TEM, HRTEM, HAADF, EDX mapping and SAED images of 3D p-CNG-M: Au (B(a-d)), Pd (C(a-d)) and Pt (D(a-d)). The up-inserts of B-D(a) are particle size distributions of cocatalysts, and the down-inserts are their SEM images. The inserts of B-D(b) are the partial magnifications of their HRTEM images.

Fig.3 (a-c) XPS high-resolution spectra of fresh and recovered 3D p-CNG-M (Au, Pd, Pt) composite catalysts, and (d-g) N₂ adsorption-desorption isotherms of 3D p-CNG skeleton and 3D p-CNG-M (Au, Pd, Pt) composite catalysts.

Fig.4 (a) HER kinetic curves, (b) average HER rates, (f) durability and (g) recycling performances of optimal 3D p-CNG-M (Au, Pd, Pt) composite catalysts. (c-e) Investigation of catalyst dosage to the HER performance of optimal 3D p-CNG-M (Au, Pd, Pt) composite catalysts. (h) HER performances of optimal 3D p-CNG-M (Au, Pd, Pt) composite catalysts in different pH values.

Fig.5 (a) UV-vis absorption spectra, (c) PL spectra, (d) TRPL spectra, (e) EIS curves (in dark and under photoinduction (L)), (f) LSV polarization curves (with interrupted photoinduction) and (g) Tafel polarization curves of 3D p-CNG skeleton and optimal 3D p-CNG-M (Pt, Pd, Au) composite catalysts. (b) Magnification of UV-vis absorption spectra of optimal 3D p-CNG (Au, Pd, Pt) composite catalysts during 450～650 nm.

Fig.6 (a) Mott-Schottky plots of 3D p-CNG skeleton and optimal 3D p-CNG-M (Au, Pd, Pt) composite catalysts. (b) VBM-XPS spectrum and (c) (ahν)^n/2-hν pattern of 2D g-C₃N₄ NSs. (d) Band structures and electron transfer mechanisms of optimal 3D p-CNG-M (Au, Pd, Pt) composite catalysts.

參考文獻(xiàn)：

[1] W. Wang, M. Xu, X. Xu, W. Zhou, Z. Shao, Angew. Chemie. Int. Ed. 59 (2019) 136–152.

[2] W. Niu, Y. Yang, ACS Energy Lett. 3 (2018) 2796–2815.

[3] Z. Zhou, Z. Pei, L. Wei, S. Zhao, X. Jian, Y. Chen, Energy Environ. Sci. 13 (2020) 3185–3206.

[4] P. Kuang, M. Sayed, J. Fan, B. Cheng, J. Yu, Adv. Energy Mater. 10 (2020) 1903802.

[5] L. Shi, X. Ren, Q. Wang, Y. Li, F. Ichihara, H. Zhang, Y. Izumi, L. Ren, W. Zhou, Y. Yang, J. Ye, Small 16 (2020) 2002356.

作者簡介：

編輯：黨妍妍          審核：李偉