Citation: Shi-Yu Lu, Wenzhao Dou, Jun Zhang, Ling Wang, Chunjie Wu, Huan Yi, Rong Wang, Meng Jin. 优化结晶度的CrS/CoS₂少层异质结非晶/晶态界面耦合增强水裂解和甲醇辅助节能制氢[J]. Acta Physico-Chimica Sinica, ;2024, 40(8): 230802. doi: 10.3866/PKU.WHXB202308024 shu

优化结晶度的CrS/CoS₂少层异质结非晶/晶态界面耦合增强水裂解和甲醇辅助节能制氢

Shi-Yu Lu ^1,, ,
Wenzhao Dou ² ,
Jun Zhang ¹ ,
Ling Wang ² ,
Chunjie Wu ² ,
Huan Yi ² ,
Rong Wang ^1,, ,
Meng Jin ^1,,

1.
College of Metallurgy and Materials Engineering, Chongqing University of Science and Technology, Chongqing 401331, China;
2.
College of Chemistry and Chemical Engineering, Chongqing University of Science and Technology, Chongqing 401331, China

Corresponding author: Shi-Yu Lu, Rong Wang, Meng Jin,
Received Date: 15 August 2023
Revised Date: 26 September 2023
Accepted Date: 27 September 2023

Fund Project: The project was supported by the Young Elite Scientists Sponsorship Program by CAST (2021QNRC001), Natural Science Foundation of Chongqing (CSTB2022NSCQ-MSX0557, cstc2020jcyj-msxmX0670, 2023NSCQ-MSX3724), Talent Introduction of Chongqing University of Science and Technology (ckrc2021050, ckrc20230401, ckrc2021053), Science and Technology Research Program of Chongqing Municipal Education Commission (KJQN202001525, KJQN202201532, KJQN202301542), National Natural Science Foundation of China (22109016) and Open Research Fund of CNMGE Platform & NSCC-TJ (CNMGE2023016).

由于电催化剂中的非晶区和结晶区具有不同的物理化学性质，因此非晶化/结晶化工程成为提高电解水催化动力学的重要策略。然而，在微观环境中有效地调控催化剂的结晶度仍然是一个严峻的挑战。本文介绍了一种可调节结晶度的新型CrS/CoS₂异质结构，该异质结对氢气析出反应(HER)和氧气析出反应(OER)都具有高效的催化活性。Cr―S―Co键的重新分配引起的d带中心移动有助于调节中间体H*和OOH*在催化剂表面的吸附能力，从而优化HER和OER的决速步骤。在最佳条件下，非晶态CrS和高度结晶的CoS₂异质结(A-CrS/HC-CoS₂)在HER和OER均表现出优异的催化活性，分别为90.6 mV (10 mA∙cm⁻²，HER)和370.5 mV (50 mA∙cm⁻²，OER)。非晶/高晶结构有利于A-CrS/HC-CoS₂在水电解过程中的结构和成分演变，因此具有出色的稳定性。作为甲醇辅助节能制氢装置中的双功能催化剂，A-CrS/HC-CoS₂仅需1.51 V的低槽电压即可达到10 mA∙cm⁻²的电流密度，证明其是理想的金属基催化剂的候选材料。本研究为双功能过渡金属化合物电催化剂在非晶态/晶态异质结构中通过结晶度调控来提高催化活性和稳定性提供了重要启示。
- Amorphous-crystalline interface,
- Heterostructure,
- Crystalline degree modulation,
- Water-splitting,
- Energy-saving hydrogen device
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优化结晶度的CrS/CoS2少层异质结非晶/晶态界面耦合增强水裂解和甲醇辅助节能制氢

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通讯作者: 陈斌, bchen63@163.com

优化结晶度的CrS/CoS₂少层异质结非晶/晶态界面耦合增强水裂解和甲醇辅助节能制氢