碳量子点/TiO<sub>2</sub> S型异质结的能带和吸附工程促进光催化CO<sub>2</sub>甲烷化

引用本文: 王文龙, 郝文韬, 何浪, 乔佳, 李宁, 陈朝秋, 覃勇. 碳量子点/TiO₂ S型异质结的能带和吸附工程促进光催化CO₂甲烷化[J]. 物理化学学报, 2025, 41(9): 100116. doi: 10.1016/j.actphy.2025.100116 shu

Citation: Wenlong Wang, Wentao Hao, Lang He, Jia Qiao, Ning Li, Chaoqiu Chen, Yong Qin. Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation[J]. Acta Physico-Chimica Sinica, 2025, 41(9): 100116. doi: 10.1016/j.actphy.2025.100116 shu

碳量子点/TiO₂ S型异质结的能带和吸附工程促进光催化CO₂甲烷化

王文龙 ^{1, 2,} ,
郝文韬 ^{2, 3,} ,
何浪 ^{2,
,} ,
乔佳 ^2, ,
李宁 ^{1,
,} ,
陈朝秋 ^{2,
,} ,
覃勇 ^2,

1.
中北大学能源与动力工程学院, 煤与煤层气共采全国重点实验室, 山西太原 030051
2.
中国科学院山西煤炭化学研究所, 煤炭高效低碳利用全国重点实验室, 山西太原 030001
3.
中国科学院大学, 北京 10049

通讯作者: 何浪, helang@sxicc.ac.cn; 李宁, lnlong2834@yeah.net; 陈朝秋, chenchaoqiu@sxicc.ac.cn

基金项目:
国家自然科学基金 22372190

中国科学院山西煤炭化学研究所 SCJC-2023-20

山西省科技创新人才团队(领军)专项基金 202304051001007

2023年度国家资助博士后研究人员计划(C档) GZC20232815

中国博士后科学基金 2024M753358

中国博士后科学基金 2024M763394

摘要: S型异质结光催化剂因同时具有优异的光生载流子分离效率和较强的氧化还原能力，而被广泛应用于光催化二氧化碳(CO₂)还原制高价值化学品(如甲烷)中。碳量子点(Carbon dots，CDs)材料具有能带结构和吸光范围可调的独特优势，可与常用半导体材料(如氧化钛，TiO ₂)形成有效S型异质结光催化剂。然而，碳量子点能带结构和表面吸附性质在调控CDs/TiO₂的异质结构型、载流子分离和传输动力学、以及CO₂活化和还原产物选择性中的重要作用仍缺乏深入研究。本文通过改变CDs的碳源，包括低阶煤沥青(C-GQDs，1.75 nm)、葡萄糖(G-CQDs，1.84 nm)、丙酮(CQDs-X，1.82 nm)和炭黑(GQDs-A，1.92 nm)，构建了四种CDs/TiO₂异质结光催化剂，并将其用于光催化CO₂甲烷化反应。研究发现，CDs/TiO₂异质结类型、光生电荷载流子的转移路径、迁移和分离效率、CO₂的吸附和活化能力以及还原产物的选择性与CDs的能带结构和表面吸附性质密切相关。CDs的引入显著增强了TiO₂光利用的能力，其中，以低价煤沥青为碳源构建的C-GQDs/TiO₂ S型异质结具有最高的CH₄生成速率，达到32.7 μmol·g⁻¹·h⁻¹，是单一TiO₂的6.3倍，并且显著高于其它三种异质结，分别是GQDs-A/TiO₂、CQDs-X/TiO₂和G-CQDs/TiO₂的3.8、2.7和2.3倍。该催化剂还具有72.6%的高电子基CH₄选择性和98.1%的烃类产物选择性(CH₄，C₂H₆，C₂H₄和C₃H₈)。相反地，其它三种碳源CDs(GQDs-A、CQDs-X和G-CQDs)的引入导致CH₄选择性大幅下降(均小于40.0%)。原位XPS和程序升温脱附实验结果表明，C-GQDs/TiO₂高的甲烷生成速率和选择性可归因于其独特的S型异质结结构、较高的还原电势和匹配的CO₂和H₂O吸附活化能力。这项研究为CDs/TiO₂光催化剂在S型异质结电子传递途径的驱动下将CO₂高效光还原为CH₄提供了独特的见解。

关键词:

English

Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation

Wenlong Wang ^{1, 2,} ,
Wentao Hao ^{2, 3,} ,
Lang He ^{2,
,} ,
Jia Qiao ^2, ,
Ning Li ^{1,
,} ,
Chaoqiu Chen ^{2,
,} ,
Yong Qin ^2,

1.
School of Energy and Power Engineering & State Key Laboratory of Coal and CBM Co-Mining, North University of China, Taiyuan 030051, Shanxi Province, China
2.
State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan 030001, Shanxi Province, China
3.
University of Chinese Academy of Sciences, Beijing 100049, China

Corresponding author: Email: helang@sxicc.ac.cn (L.H.); Email: lnlong2834@yeah.net (N.L.); Email: chenchaoqiu@sxicc.ac.cn (C.C.)

Received Date: 27 April 2025
Accepted Date: 10 June 2025
Revised Date: 09 June 2025
Available Online: 15 September 2025
Fund Project:
the National Natural Science Foundation of China

ICC CAS

the special fund for Science and Technology Innovation Teams of Shanxi Province

the Postdoctoral Fellowship Program of CPSF

China Postdoctoral Science Foundation

China Postdoctoral Science Foundation

Abstract: S-scheme heterojunctions have garnered significant interest in photocatalytic CO₂ conversion to valuable products (e.g., CH₄) due to their enhanced charge separation and robust redox capabilities. Carbon dots (CDs), with their tunable band structures and light absorption ranges, show particular promise in constructing efficient S-scheme photocatalytic systems. Nevertheless, the critical roles of CDs' band alignment and surface adsorption properties in determining heterojunction configuration, charge carrier kinetics, and ultimately CO₂ activation/product selectivity distribution remain insufficiently explored. Herein, we construct four CDs/TiO₂ heterojunctions using CDs synthesized from varied carbon sources, in which S-scheme heterojunctions were successfully constructed based on cost-effective coal pitch (C-GQDs, 1.75 nm), glucose (G-CQDs, 1.84 nm), and acetone (CQDs-X, 1.82 nm) carbon sources, whereas Type-Ⅰ heterojunctions were formed by carbon black based CDs (GQDs-A, 1.92 nm). Systematic investigations reveal that both the band structure and adsorption characteristics of CDs play important roles in the charge transfer path and separation efficiency, CO₂ adsorption and activation capacities, and product selectivity in photocatalytic CO₂ reduction. Remarkably, the introduction of CDs significantly broadens the photo-response range compared to fresh TiO₂, and in particular, the C-GQDs/TiO₂ exhibits exceptional performance with a CH₄ production rate of 32.7 μmol·g⁻¹·h⁻¹, surpassing TiO₂ by 6.3-fold and outperforming GQDs-A/TiO₂, CQDs-X/TiO₂, and G-CQDs/TiO₂ by factors of 3.8, 2.7, and 2.3, respectively. This heterojunction simultaneously achieves 72.6% CH₄ selectivity and 98.1% hydrocarbons selectivity (encompassing CH₄, C₂H₆, C₂H₄, and C₃H₈). In contrast, composites incorporating GQDs-A, CQDs-X, or G-CQDs exhibit substantially diminished CH₄ selectivity (< 40.0%). The high CH₄ production rate and selectivity of C-GQDs/TiO₂ can be attributed to its unique S-scheme heterojunction structure, higher reduction potential, and well-matched CO₂ and H₂O adsorption and activation capabilities. This study provides unique insights into the efficient photoreduction of CO₂ to CH₄ driven by the S-scheme heterojunction electron transfer pathway in CDs/TiO₂ photocatalysts.

Key words:

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通讯作者: 何浪, helang@sxicc.ac.cn; 李宁, lnlong2834@yeah.net; 陈朝秋, chenchaoqiu@sxicc.ac.cn

English

Bandgap and adsorption engineering of carbon dots/TiO₂ S-scheme heterojunctions for enhanced photocatalytic CO₂ methanation

Corresponding author: Email: helang@sxicc.ac.cn (L.H.); Email: lnlong2834@yeah.net (N.L.); Email: chenchaoqiu@sxicc.ac.cn (C.C.)

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通讯作者: 何浪, helang@sxicc.ac.cn; 李宁, lnlong2834@yeah.net; 陈朝秋, chenchaoqiu@sxicc.ac.cn

English

Bandgap and adsorption engineering of carbon dots/TiO2 S-scheme heterojunctions for enhanced photocatalytic CO2 methanation

Corresponding author: Email: helang@sxicc.ac.cn (L.H.); Email: lnlong2834@yeah.net (N.L.); Email: chenchaoqiu@sxicc.ac.cn (C.C.)

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通讯作者: 陈斌, bchen63@163.com

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