Ti3C2 MXene纳米片上原位生长的Cd0.5Zn0.5S纳米棒实现高效可见光催化析氢

引用本文: 李钦, 张慧慧, 顾华军, 崔园园, 高瑞华, 戴维林. Ti₃C₂ MXene纳米片上原位生长的Cd_0.5Zn_0.5S纳米棒实现高效可见光催化析氢[J]. 物理化学学报, 2025, 41(4): 100031. doi: 10.3866/PKU.WHXB202402016 shu

Citation: Qin Li, Huihui Zhang, Huajun Gu, Yuanyuan Cui, Ruihua Gao, Wei-Lin Dai. In situ Growth of Cd_0.5Zn_0.5S Nanorods on Ti₃C₂ MXene Nanosheet for Efficient Visible-Light-Driven Photocatalytic Hydrogen Evolution[J]. Acta Physico-Chimica Sinica, 2025, 41(4): 100031. doi: 10.3866/PKU.WHXB202402016 shu

Ti₃C₂ MXene纳米片上原位生长的Cd_0.5Zn_0.5S纳米棒实现高效可见光催化析氢

李钦 ^1, ,
张慧慧 ^1, ,
顾华军 ^1, ,
崔园园 ^3, ,
高瑞华 ^{2,
,} ,
戴维林 ^{1,
,}

1.
复旦大学化学系, 上海市分子催化与创新材料重点实验室, 上海 200433;
2.
复旦大学高分子科学系, 聚合物分子工程国家重点实验室, 上海 200433;
3.
岛津中国有限公司, 上海 200436

通讯作者: 高瑞华, E-mail: ruihuagao@fudan.edu.cn; 戴维林, E-mail: wldai@fudan.edu.cn

基金项目:
科技部国家重点研发计划(2021YFA1501404)，上海市自然科学基金(22ZR1404200)，国家自然科学基金(21373054)以及上海市科学技术委员会专项经费(19DZ2270100).

摘要: 在能源短缺和环保优先的背景下，光催化制氢是将太阳能转化为化学能的重要途径之一。有效提高光生载流子的分离效率对于设计具有优异析氢活性的光催化剂至关重要。本研究采用一步原位水热法构建了由Cd_0.5Zn_0.5S纳米棒和Ti₃C₂ MXene纳米片组成的二元异质结光催化剂。当Ti₃C₂ MXene的含量为0.5 wt% (质量分数)时，光催化产氢的最大速率为15.56 mmol∙g⁻¹∙h⁻¹，是纯Cd_0.5Zn_0.5S的2.56倍。经过5次催化循环后，光催化活性没有显著下降。该材料在350 nm紫外光下展现出最高的AQE为18.4%。此外，基于X射线光电子能谱(XPS)、原位光照XPS、飞秒瞬态吸收光谱、密度泛函理论(DFT)计算和光催化活性实验，我们提出了MXene/Cd_0.5Zn_0.5S复合材料的电荷转移和光催化制氢机理。我们的研究表明，引入不含贵金属的MXene材料可以有效地帮助光生电子的转移。这项工作展示了MXene材料在构建高效低成本的制氢光催化剂方面的潜力。

关键词:

English

In situ Growth of Cd_0.5Zn_0.5S Nanorods on Ti₃C₂ MXene Nanosheet for Efficient Visible-Light-Driven Photocatalytic Hydrogen Evolution

Qin Li ^1, ,
Huihui Zhang ^1, ,
Huajun Gu ^1, ,
Yuanyuan Cui ^3, ,
Ruihua Gao ^{2,
,} ,
Wei-Lin Dai ^{1,
,}

1.
Department of Chemistry and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai 200433, China;
2.
State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200433, China;
3.
Shimadzu China Co LTD, Shanghai 200436, China

Corresponding author: Ruihua Gao, ; Wei-Lin Dai,

Received Date: 19 February 2024
Accepted Date: 03 April 2024
Revised Date: 03 April 2024
Fund Project:
This work was financially supported by the National Key Research and Development Program of China (2021YFA1501404), Natural Science Foundation of Shanghai (22ZR1404200), National Natural Science Foundation of China (21373054), and Natural Science Foundation of Shanghai Science and Technology Committee (19DZ2270100).

Abstract: Against the backdrop of energy scarcities and ecological concerns, the process of photocatalytic hydrogen evolution emerges as a critical method for transforming solar energy into chemical energy. Central to this technology is the crafting of photocatalysts that are not only efficient and durable but also economically viable. The key to creating photocatalysts that boast superior hydrogen production capabilities lies in enhancing the separation and transfer of photo-generated electrons and holes. This study introduces a binary heterojunction photocatalyst, featuring a combination of Cd_0.5Zn_0.5S and Ti₃C₂ MXene, synthesized via an in situ hydrothermal method. In the composite, slender Cd_0.5Zn_0.5S nanorods are uniformly coated over the surface of single layer Ti₃C₂ nanosheets, forming a Schottky heterojunction at the material interface. This structure enhances the separation efficiency of photo-generated electrons and holes, thereby improving the utilization of light. With 0.5 wt% (mass fraction) of Ti₃C₂ MXene incorporated, we observed a peak photocatalytic H₂ generation rate of 15.56 mmol∙g⁻¹∙h⁻¹, outperforming the baseline Cd_0.5Zn_0.5S by 2.56 times. Notably, the photocatalytic efficiency remained largely unchanged after five cycles. This composite achieved the highest apparent quantum efficiency (AQE) of 18.4% when exposed to 350 nm UV light. Various characterization techniques, including in situ X-ray photoelectron spectroscopy (XPS) and femtosecond transient absorption (fs-TA) spectroscopy, along with density functional theory (DFT) calculations, have further substantiated that the formation of a Schottky heterojunction at the interface is crucial for enhancing the photocatalytic hydrogen evolution performance of the composite material. This paper demonstrates the effectiveness of the novel carbon based material MXene as a co-catalyst for improving the performance of photocatalysts and offers a viable approach for the construction of MXene-containing photocatalytic hydrogen evolution catalysts.

Key words:

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沈阳化工大学材料科学与工程学院沈阳 110142

Ti₃C₂ MXene纳米片上原位生长的Cd_0.5Zn_0.5S纳米棒实现高效可见光催化析氢

通讯作者: 高瑞华, E-mail: ruihuagao@fudan.edu.cn; 戴维林, E-mail: wldai@fudan.edu.cn

English

In situ Growth of Cd_0.5Zn_0.5S Nanorods on Ti₃C₂ MXene Nanosheet for Efficient Visible-Light-Driven Photocatalytic Hydrogen Evolution

Corresponding author: Ruihua Gao, ; Wei-Lin Dai,

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