太阳光驱动界面局域光热催化实现非食用油高效转化制备生物柴油

doi:10.1016/S1872-2067(26)65087-5

催化学报 ›› 2026, Vol. 87: 156-169.DOI: 10.1016/S1872-2067(26)65087-5

太阳光驱动界面局域光热催化实现非食用油高效转化制备生物柴油

周恒^a, 洪龙飞^b, 张艳^a, 周雨悦^a, 储升^b^,^*(), 张会岩^b^,^*(), 李慧^c^,^d, 马天翼^c^,^d^,^*(), 张衡^a^,^*()

^a 贵州大学精细化工研究开发中心, 绿色农药全国重点实验室, 生物质资源综合利用国家地方联合工程实验室, 贵州贵阳 550025, 中国
^b 东南大学能源与环境学院, 能源热转换及其过程测控教育部重点实验室, 江苏南京 210096, 中国
^c 皇家墨尔本理工大学科学学院, 原子材料与纳米制造中心, 墨尔本, 澳大利亚
^d 未来设施园艺智能能效产业转型中心, 墨尔本, 澳大利亚

收稿日期:2025-10-04 接受日期:2026-01-04 出版日期:2026-08-18 发布日期:2026-06-24
通讯作者: ^*电子信箱: schu@seu.edu.cn (储升),
hyzhang@seu.edu.cn (张会岩),
tianyi.ma@rmit.edu.au (马天翼),
hzhang23@gzu.edu.cn (张衡).
基金资助:
国家自然科学基金(32302418);国家自然科学基金(52522610);国家杰出青年科学基金(52425607);贵州省科技创新平台科研项目(CXPTXM [2025] 012);中央引导地方科技发展资金项目(Qiankehezhongyindi (2024) 007);贵州省科技支撑计划(ZC [2023]330);江苏省自然科学基金(BK20240010)

Efficient solar-simulated-driven valorization of non-edible oils for biodiesel production via interfacial localized photothermal catalysis

Heng Zhou^a, Longfei Hong^b, Yan Zhang^a, Yuyue Zhou^a, Sheng Chu^b^,^*(), Huiyan Zhang^b^,^*(), Hui Li^c^,^d, Tianyi Ma^c^,^d^,^*(), Heng Zhang^a^,^*()

^a State Key Laboratory of Green Pesticide, State-Local Joint Laboratory for Comprehensive Utilization of Biomass, Center for R&D of Fine Chemicals of Guizhou University, Guiyang 550025, Guizhou, China
^b Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing 210096, Jiangsu, China
^c Centre for Atomaterials and Nanomanufacturing (CAN), School of Science, RMIT University, Melbourne, VIC3000, Australia
^d ARC Industrial Transformation Research Hub for Intelligent Energy Efficiency in Future Protected Cropping (E2Crop), Melbourne, VIC3000, Australia

Received:2025-10-04 Accepted:2026-01-04 Online:2026-08-18 Published:2026-06-24
Supported by:
National Natural Science Foundation of China(32302418);National Natural Science Foundation of China(52522610);National Natural Science Fund for Distinguished Young Scholars of China(52425607);Guizhou Provincial S&T Innovation Platform Research Program(CXPTXM [2025] 012);Central Government Guides Local Science and Technology Development Fund Projects(Qiankehezhongyindi (2024) 007);Guizhou Provincial Key Technology R&D Program(ZC [2023]330);Natural Science Foundation of Jiangsu Province(BK20240010)

摘要/Abstract

摘要：

在全球能源转型与碳中和战略深入推进的背景下,发展安全、绿色、环保的可持续能源已成共识. 化石燃料的过度消耗加剧了能源危机与气候变化, 而以液体生物质合成的生物柴油因能完全替代化石柴油, 成为极具潜力的低碳可持续燃料解决方案. 阳光作为全球分布最广泛的清洁能源, 凭借其环境友好及温和的反应条件, 在光催化领域备受青睐. 然而, 传统半导体光催化剂普遍面临光生载流子快速重组、太阳光利用率低等瓶颈. 如何高效利用全光谱, 特别是低能量近红外光(约占总辐射量的50%)以实现非食用油的增值利用仍是重大挑战. 因此, 开发绿色高效合成生物柴油的全光谱响应光热催化体系已成为可再生能源转化领域亟待解决的关键问题.

本文以可再生纤维素为原料, 通过碱预处理得到预处理纤维素(PC), 采用柠檬酸和对甲苯磺酸协同水热法, 成功制备了无金属光热催化材料PC-SO₃H-1, 该催化剂能够利用整个太阳光谱进行高效的生物柴油生产, 仅需30 min即可达到98.29%的生物柴油产率, 显著突破热力学平衡极限. 通过扫描电镜、X射线衍射、傅里叶变换红外光谱及拉曼光谱等表征手段证实PC-SO₃H-1的成功制备. 多尺度表征结合密度泛函理论(DFT)计算揭示, PC-SO₃H-1的窄带隙赋予其良好的全光谱吸收特性(300‒1400 nm); 同时其表面丰富的-SO₃H酸性位点可强化油酸的吸附与活化, 有效克服了热力学平衡限制. 通过电化学阻抗谱、瞬态光电流响应、线性扫描伏安法和光致发光光谱系统研究了催化剂样品的光生载流子的迁移和复合行为. 结果表明, PC-SO₃H-1优化的载流子迁移动力学加速了界面局部光热效应, 推动酯化反应正向进行, 在显著提升近红外光子利用率的同时最大限度降低了体系热损失. 值得注意的是, 在经过8次循环实验后, PC-SO₃H-1仍保持优异的催化稳定性. 另外, 通过调控反应条件, 深入探讨并提出了光热催化协同生产生物柴油的机制. 红外热成像与COMSOL模拟证实, PC-SO₃H-1对近红外光的强吸收及界面局部光热效应是体系温度升高的关键原因. 吉布斯自由能计算表明, PC-SO₃H-1有效降低了速率决定步骤的活化能垒, 促进关键中间体羰基酯(C=O)的生成. 此外, 原位红外与原位拉曼表征结果直接证实, 在近红外光主导的光热催化过程中, 油酸甲酯可快速生成, 进一步佐证了所提出的反应机理.

综上, 本工作成功开发了一种高效、稳定的无贵金属光热催化体系, 克服了传统光催化技术对高能光子的依赖, 为实现全光谱太阳驱动绿色燃料的可持续生产提供了新途径, 对推进绿色能源转化领域的发展具有积极意义.

关键词: 光热催化, 生物柴油, 近红外光, 液体生物质, 酯化反应

Abstract:

Harnessing solar energy as a power source for sustainable fuel production from biomass waste presents an effective solution to energy and environmental challenges. However, efficient utilization of low-energy near-infrared (NIR) light (representing ~50% of solar irradiance) continues a critical bottleneck especially for non-edible oils valorization. Here, we report a cellulose-derived sulfonated hydrochar (PC-SO₃H-1) utilizing the full solar spectrum for highly efficient biodiesel production, achieving a remarkable biodiesel yield of 98.29% within only 30 min, which far exceeds the theoretical limit. Favorable NIR absorption of narrow bandgap PC-SO₃H-1 combined with substrate adsorption capacity enhanced by -SO₃H functionalization overcomes thermodynamic equilibrium limitations. The optimized charge transfer dynamics accelerate the interfacial localized photothermal effect, driving the esterification reaction forward while minimizing heat loss and significantly enhancing the utilization of NIR photons. Density functional theory calculations demonstrate the formation of crucial intermediate ester carbonyl groups (C=O), with PC-SO₃H-1 effectively reducing the activation energy barrier associated with the rate-limiting process. This sustainable noble metal-free photothermal catalytic system of high-efficiency overcomes the reliance of traditional photocatalysis on high-energy photons, offering novel insights into the full spectrum solar-driven production of green and renewable biofuels.

Key words: Photothermal catalysis, Biodiesel, Near-infrared light, Liquid biomass, Esterification reaction

周恒, 洪龙飞, 张艳, 周雨悦, 储升, 张会岩, 李慧, 马天翼, 张衡. 太阳光驱动界面局域光热催化实现非食用油高效转化制备生物柴油[J]. 催化学报, 2026, 87: 156-169.

Heng Zhou, Longfei Hong, Yan Zhang, Yuyue Zhou, Sheng Chu, Huiyan Zhang, Hui Li, Tianyi Ma, Heng Zhang. Efficient solar-simulated-driven valorization of non-edible oils for biodiesel production via interfacial localized photothermal catalysis[J]. Chinese Journal of Catalysis, 2026, 87: 156-169.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65087-5

https://www.cjcatal.com/CN/Y2026/V87/I8/156

图/表 6

Scheme 1. (a) Current methods for biodiesel production. (b) Traditional noble metal-based photothermal materials. (c) Elaboration of the key highlights in this work.

Fig. 1. Synthesis and characterization of target catalysts. (a) Schematic representation of the preparation for PC-SO3H-1. (b) HOMO-LUMO gap of OA. Simulated adsorption of OA at -OH (c), -COOH (d), and -SO3H (e). SEM images of PC-1 (f), PC-SO3H (g), and PC-SO3H-1 (h) (inset: the corresponding particle size distribution). (i) Element mapping images of PC-SO3H-1. XRD patterns (j) and FT-IR spectra (k) of cellulose, PC, PCC, PC-1, PC-SO3H, and PC-SO3H-1. N2 adsorption-desorption isotherms (l) and Raman spectra (m) of PC-1, PC-SO3H, and PC-SO3H-1.

Fig. 2. Optical properties and bonding structure. (a) ESP image of SGQD model. (b) UV-Vis DRS of cellulose, PC, PCC, PC-1, PC-SO3H, and PC-SO3H-1. XPS valence band spectra (c) and energy band structures (d) of PC-1, PC-SO3H, and PC-SO3H-1. (e) Spatial distribution of LUMO and HOMO orbits of GQD, CGQD, and SGQD. High-resolution C 1s (f), O 1s (g), and S 2p (h) XPS spectra of PC-1, PC-SO3H, and PC-SO3H-1. The XAS spectra of C K-edge (i) and O K-edge (j) of PC-1, PC-SO3H, and PC-SO3H-1. (k) The XAS spectra of S L-edge of PC-SO3H and PC-SO3H-1.

Fig. 3. Photoelectrochemical characterization and adsorb ability. EIS Nyquist plots (a) and transient photocurrent response curves (b) of cellulose, PC, PCC, PC-1, PC-SO3H, and PC-SO3H-1. (c) PL spectra of PC-1, PC-SO3H, and PC-SO3H-1. (d) OA adsorption properties of PC-1, PC-SO3H, and PC-SO3H-1. (e) The Eads of each adsorption site on SGQD for OA and MeOH. Model fitting of adsorption kinetics (f), internal diffusion modeling (g), and adsorption isotherm (h) of OA adsorption on PC-SO3H-1.

Fig. 4. Evaluation of photothermal catalytic performance. Infrared thermography pictures (a) and temperature change curves (b) under full spectrum irradiation of PC-1, PC-SO3H, and PC-SO3H-1. (c) COMSOL simulation results under full spectrum irradiation. (d) The variation of biodiesel yield with time under full spectrum irradiation of PC-1, PC-SO3H, and PC-SO3H-1. Infrared thermography pictures (e) and temperature elevating curves (f) under irradiation of UV-vis, NIR, and full spectrum. (g) The variation of biodiesel yield with time under different conditions (dark + heating (70 °C), UV-vis, NIR, and full spectrum) by PC-SO3H-1. (h) Arrhenius plots of PC-SO3H-1 under different light conditions. (i) Comparison of biodiesel yield performance under different light conditions (with/without cooling). (j) Reusability and 10-fold magnification experiment. (k) Comparison of catalytic activity and reaction time of different catalysts.

Fig. 5. Mechanism insights of photothermal catalytic esterification reaction. (a) Effect of scavenging agents on biodiesel yield. EPR signals depicting TEMPO-h+ (b) and DMPO-CH3O• (c) in PC-SO3H-1 photothermal catalytic esterification of OA. (d,e) In situ DRIFTS spectra during photothermal catalytic OA esterification with PC-SO3H-1 under UV-vis light irradiation, NIR light irradiation, and full spectrum. (f) Calculated reaction Gibbs free energy diagram of OA esterification (Catalyst-free, PC-1, PC-SO3H, and PC-SO3H-1). (g) Schematic diagram of catalytic mechanism enhanced by the photothermal effect.

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太阳光驱动界面局域光热催化实现非食用油高效转化制备生物柴油

Efficient solar-simulated-driven valorization of non-edible oils for biodiesel production via interfacial localized photothermal catalysis

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