当前位置：
X-MOL 学术
›
ACS Appl. Energy Mater.
›
论文详情
Our official English website, www.x-mol.net, welcomes your
feedback! (Note: you will need to create a separate account there.)
Two-Dimensional Janus van der Waals Heterojunctions SnX2@SnSSe (X = S, Se) as Promising Solar-Driven Water-Splitting Photocatalysts
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-12-15 , DOI: 10.1021/acsaem.3c02081
Meiqiu Xie 1 , Yi Shang 1 , Xiaolong Xu 1 , Xuhai Liu 2 , Hui Li 1 , Xing’ao Li 1
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2023-12-15 , DOI: 10.1021/acsaem.3c02081
Meiqiu Xie 1 , Yi Shang 1 , Xiaolong Xu 1 , Xuhai Liu 2 , Hui Li 1 , Xing’ao Li 1
Affiliation
|
Constructing stable two-dimensional (2D) van der Waals heterojunctions (vdWHs) as potential high-efficiency photocatalysts with an intrinsic electric field and tunable properties is of vital importance to explore direct solar-driven water splitting without sacrificial agents and cocatalysts. Herein, 16 designed 2D MX2@MSSe vdWHs (M = Ge, Sn; X = S, Se) by assembling MX2 and Janus MSSe monolayers with classic T- and H-phases are comprehensively studied by density functional theory. Eight of the T-MX2@MSSe vdWHs are considered to be more stable than the corresponding H-phase vdWHs according to ab initio molecular dynamics calculations. The T-GeX2@GeSSe and T-SnX2@SnSSe vdWHs exhibit semiconductor properties, with tunable band gaps of 0.14–0.49 and 1.20–1.53 eV, respectively. Remarkably, the band alignments of T-SSnS@SSnSe, T-SSnS@SeSnS, T-SeSnSe@SSnSe, and T-SeSnSe@SeSnS vdWHs under an intrinsic electric field straddle the reaction potential of O2/H2O and H+/H2 when participating in photocatalytic processes. Additionally, such four T-Sn-based vdWHs exhibit ∼104 cm2 V–1 s–1 carrier mobilities, and the appreciable difference between electron and hole mobilities could render the rapid migration and weaken the recombination of photogenerated carriers. Meanwhile, the T-SnX2@SnSSe vdWHs possess broader visible light absorptions than those of their monolayer counterparts. In view of the outstanding characteristics for overall water splitting, the photocatalytic mechanisms of T-SnX2@SnSSe vdWHs have been clarified. Moreover, the chemical driving force of the photogenerated carriers in T-SnX2@SnSSe vdWHs can apparently facilitate redox reactions. The hydrogen reduction of T-SnX2@SnSSe vdWHs along with the water oxidation of T-SSnS@SSnSe and T-SeSnSe@SSnSe vdWHs can occur spontaneously under light irradiation. This work regarding 2D group IV metal chalcogenides could pave the way for competent photocatalyst system construction.
中文翻译：
二维 Janus van der Waals 异质结 SnX2@SnSSe (X = S, Se) 作为有前景的太阳能驱动水分解光催化剂
构建稳定的二维（2D）范德华异质结（vdWH）作为具有固有电场和可调特性的潜在高效光催化剂对于探索无需牺牲剂和助催化剂的直接太阳能驱动水分解至关重要。在此，16人通过密度泛函理论对具有经典T相和H相的MX 2和Janus MSSe单分子层组装设计了2D MX 2 @MSSe vdWHs (M = Ge, Sn; X = S, Se) 。根据从头算分子动力学计算，八个 T-MX 2 @MSSe vdWH 被认为比相应的 H 相 vdWH 更稳定。T-GeX 2 @GeSSe 和 T-SnX 2 @SnSSe vdWH 表现出半导体特性，可调带隙分别为 0.14–0.49 和 1.20–1.53 eV。值得注意的是，T-SSnS@SSnSe、T-SSnS@SeSnS、T-SeSnSe@SSnSe 和 T-SeSnSe@SeSnS vdWH 在本征电场下的能带排列横跨 O 2 /H 2 O 和 H +的反应电位/H 2当参与光催化过程时。此外，这四种T-Sn基vdWH表现出~10 4 cm 2 V –1 s –1载流子迁移率，电子和空穴迁移率之间的显着差异可能导致光生载流子的快速迁移并削弱其复合。同时，T-SnX 2 @SnSSe vdWH 比单层同类材料具有更广泛的可见光吸收。鉴于整体水分解的突出特性，T-SnX 2 @SnSSe vdWHs的光催化机制已被阐明。此外，T-SnX 2 @SnSSe vdWHs中光生载流子的化学驱动力可以明显促进氧化还原反应。T-SnX 2 @SnSSe vdWHs的氢还原以及 T-SSnS@SSnSe 和 T-SeSnSe@SSnSe vdWHs 的水氧化可以在光照射下自发发生。这项关于二维 IV 族金属硫属化物的工作可以为有效的光催化剂系统构建铺平道路。
更新日期：2023-12-15
中文翻译：
二维 Janus van der Waals 异质结 SnX2@SnSSe (X = S, Se) 作为有前景的太阳能驱动水分解光催化剂
构建稳定的二维（2D）范德华异质结（vdWH）作为具有固有电场和可调特性的潜在高效光催化剂对于探索无需牺牲剂和助催化剂的直接太阳能驱动水分解至关重要。在此，16人通过密度泛函理论对具有经典T相和H相的MX 2和Janus MSSe单分子层组装设计了2D MX 2 @MSSe vdWHs (M = Ge, Sn; X = S, Se) 。根据从头算分子动力学计算，八个 T-MX 2 @MSSe vdWH 被认为比相应的 H 相 vdWH 更稳定。T-GeX 2 @GeSSe 和 T-SnX 2 @SnSSe vdWH 表现出半导体特性，可调带隙分别为 0.14–0.49 和 1.20–1.53 eV。值得注意的是，T-SSnS@SSnSe、T-SSnS@SeSnS、T-SeSnSe@SSnSe 和 T-SeSnSe@SeSnS vdWH 在本征电场下的能带排列横跨 O 2 /H 2 O 和 H +的反应电位/H 2当参与光催化过程时。此外，这四种T-Sn基vdWH表现出~10 4 cm 2 V –1 s –1载流子迁移率，电子和空穴迁移率之间的显着差异可能导致光生载流子的快速迁移并削弱其复合。同时，T-SnX 2 @SnSSe vdWH 比单层同类材料具有更广泛的可见光吸收。鉴于整体水分解的突出特性，T-SnX 2 @SnSSe vdWHs的光催化机制已被阐明。此外，T-SnX 2 @SnSSe vdWHs中光生载流子的化学驱动力可以明显促进氧化还原反应。T-SnX 2 @SnSSe vdWHs的氢还原以及 T-SSnS@SSnSe 和 T-SeSnSe@SSnSe vdWHs 的水氧化可以在光照射下自发发生。这项关于二维 IV 族金属硫属化物的工作可以为有效的光催化剂系统构建铺平道路。
京公网安备 11010802027423号