第二代生物柴油制备的多相催化剂的结构设计及研究进展

doi:10.6023/A22040189

化学学报 ›› 2022, Vol. 80 ›› Issue (9): 1322-1337.DOI: 10.6023/A22040189 上一篇下一篇

综述

第二代生物柴油制备的多相催化剂的结构设计及研究进展

田钊炜, 达伟民, 王雷, 杨宇森^*(), 卫敏

北京化工大学化学学院化工资源有效利用国家重点实验室北京 100029

投稿日期:2022-04-26 发布日期:2022-07-01
通讯作者: 杨宇森

作者简介:

田钊炜, 女, 北京化工大学在读研究生, 2021年6月于北京化工大学材料科学与工程学院材料科学与工程专业, 获得学士学位, 随后加入北京化工大学化工资源有效利用国家重点实验室卫敏教授课题组, 主要研究方向为第二代生物柴油的制备和发展.

杨宇森, 博士, 副教授, 硕士生导师. 2019年于北京化工大学获得化学工程与技术博士学位, 师从卫敏教授. 2019年至今在北京化工大学化工资源有效利用国家重点实验室从事多相催化研究, 主要研究方向: (1)生物质平台分子的定向催化转化; (2)可再生资源途径制氢、氢气精制与高效利用. 目前, 已发表SCI研究论文40余篇. 以第一(含共一)作者和共同通讯作者在Nat. Commun.、ACS Catal.、Appl. Catal. B: Environ.、J. Catal.、Green Chem.、《化学学报》及《化工学报》等期刊发表学术论文25篇(其中IF>10的16篇), 申请国家发明专利6件(其中获得授权1件).

卫敏, 女, 教授, 博士生导师. 2001年于北京大学获理学博士学位. 2008年佐治亚理工学院访问学者. 2001年至今于北京化工大学从事插层化学与功能材料研究. 研究方向: (1)插层结构功能材料的结构设计、组装与性能调控; (2)新型催化材料的结构设计和性能研究. 近5年以通讯作者在J. Am. Chem. Soc.、Angew. Chem., Int. Ed.、Nat. Commun.等刊物发表SCI收录研究论文90余篇; 他引11700余次. 2016年入选英国皇家化学会会士; 现担任Sci. Bull.期刊副主编, 催化学报编委. 获2012年国家杰出青年基金资助. 获2015年中国石油和化学工业联合会科技进步一等奖. 入选2017年度科技部中青年科技创新领军人才和国家百千万人才工程, 被授予“有突出贡献中青年专家”称号. 获2018年第十五届中国青年科技奖.

基金资助:
北京自然科学基金(2212012); 国家自然科学基金(22172006); 国家自然科学基金(21521005); 国家自然科学基金(22102006); 国家重点研发计划(2021YFC2103501); 中央高校基本科研业务费(XK1803-05)

Structural Design and Research Progress of Heterogeneous Catalysts for the Preparation of Second Generation Biodiesel

Zhaowei Tian, Weimin Da, Lei Wang, Yusen Yang(), Min Wei

State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029

Received:2022-04-26 Published:2022-07-01
Contact: Yusen Yang
Supported by:
Beijing Natural Science Foundation(2212012); National Natural Science Foundation of China(22172006); National Natural Science Foundation of China(21521005); National Natural Science Foundation of China(22102006); National Key Research and Development Program(2021YFC2103501); Fundamental Research Funds for the Central Universities(XK1803-05)

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摘要/Abstract

生物柴油是一种重要的可再生清洁能源, 特别是经催化加氢脱氧等系列过程制备的第二代生物柴油, 在成分上与石油基燃料相似, 有望成为一种替代传统化石燃料的绿色能源. 在合成第二代生物柴油的研究中, 设计与制备兼具高活性与高稳定性的加氢脱氧多相催化剂是关键问题. 近年来, 研究者对于催化剂的种类与应用进行了探索, 并取得了一定的进展. 详细分析了加氢脱氧制备第二代生物柴油反应原料及反应参数、反应器对生产路径和产能的影响, 并对反应机理进行了介绍; 进一步从双金属位点、金属-酸性位点及金属-空位协同作用三个方面对催化剂结构设计进行了讨论和分析; 最后, 对第二代生物柴油领域的未来发展趋势进行了展望.

关键词: 生物质, 生物柴油, 加氢脱氧, 多相催化剂, 协同作用

Biodiesel is an important renewable and clean energy, especially the second-generation of biodiesel prepared by a series of processes such as catalytic hydrodeoxygenation. It is similar to petroleum-based fuels in composition, and is expected to become a green energy alternative to traditional fossil fuels. In the study of the synthesis of the second generation of biodiesel, the design and preparation of hydrodeoxygenation heterogeneous catalysts with high activity and stability are the key issues. In recent years, many studies have been reported on the types and applications of catalysts, and some research progress has been made. The effects of reaction materials, reaction parameters and reactor on the production path and capacity of the second generation biodiesel prepared by hydrodeoxygenation were surveyed in detail, and the reaction mechanism was introduced. Then regulation strategies of hydrodeoxygenation catalysts are discussed and analyzed from three aspects: bimetallic sites, metal-acidic sites and metal-vacancy synergistic effect. In the final section, future development opportunities and challenges for the second-generation biodiesel are prospected.

Key words: biomass, biodiesel, hydrodeoxygenation, heterogeneous catalyst, synergistic effect

引用此文

田钊炜, 达伟民, 王雷, 杨宇森, 卫敏. 第二代生物柴油制备的多相催化剂的结构设计及研究进展[J]. 化学学报, 2022, 80(9): 1322-1337.

Zhaowei Tian, Weimin Da, Lei Wang, Yusen Yang, Min Wei. Structural Design and Research Progress of Heterogeneous Catalysts for the Preparation of Second Generation Biodiesel[J]. Acta Chimica Sinica, 2022, 80(9): 1322-1337.

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图/表 10

图1. 加氢脱氧制备第二代生物柴油催化剂的结构设计示意图

Figure 1. Schematic diagram of structure design of hydrodeoxygenation catalysts for the synthesis of second-generation biodiesel

图2. (a)硬脂酸、油酸、亚油酸在PtSnx/C催化剂上的转化率以及对不同产物的产率[41]、(b)不同碳数的脂肪酸在Pt/MWNTs催化剂上的转化率和脱羧产物的选择性[42]以及(c)反应温度和氢气压力对烷烃产量的影响[28]

Figure 2. (a) Molar yields of products and conversion of stearic acid, oleic acid and linoleic acid over PtSnx/C catalysts[41], (b) conversion and selectivity for different fatty acids decarboxylation over Pt/MWNTs[42], and (c) temperature and pressure effect on hydrocarbon yield[28]

图3. 不同原料加氢脱氧制备第二代生物柴油[43]

Figure 3. Preparation of second generation biodiesel by hydrodeoxygenation of different feedstocks[43]

图4. 不饱和脂肪酸甲酯的加氢脱氧反应路径示意图

Figure 4. Schematic diagram of hydrodeoxygenation reaction pathway of unsaturated fatty acid methyl ester

图5. (a)脂肪酸在Ru(0001)面上进行脱氧反应不同步骤吸附模型[51]、(b) Ni/MoOx催化剂脱氧反应机理图[56]、(c) Ni/ZrO2催化硬脂酸脱羰反应机理图[38]和(d) Pd基催化剂进行脂肪酸甲酯DCO2路径脱氧反应[60]

Figure 5. (a) Adsorption model of fatty acid on Ru(0001) surface by different deoxidation steps[51], (b) mechanism of deoxidation reaction over Ni/MoOx catalyst[56], (c) mechanism diagram of decarbonylation of stearic acid over Ni/ZrO2 catalyst[38] and (d) DCO2 pathway deoxidation of fatty acid methyl ester over Pd-based catalyst[60]

图6. (a)不同Cu/Ni原子比的Cu-Ni合金催化剂的XRD图谱、H2-TPR图像、Cu 2p3/2轨道的XPS光谱、CO化学吸附的漫反射傅里叶变换红外光谱和(b)乙烯、丙烷和乙酸在CuAl、CuNi2Al和NiAl上的程序升温脱附图像[76]

Figure 6. (a) XRD patterns, H2-TPR profiles, XPS spectra for Cu 2p3/2 and DRIFTS-IR spectra with CO probes of Cu-Ni alloy catalysts with different Cu/Ni atomic ratio and (b) temperature-programmed desorption of C2H4, C3H8 and CH3COOH on CuAl, CuNi2Al and NiAl[76]

图7. (a) NixFey/SiO2催化剂的H2-TPR谱图、CO-FTIR谱图及XPS谱图和(b)乙酸、H、OH在洁净表面吸附构型以及Ni(111)面乙酸脱氧的势能图[83]

Figure 7. (a) H2-TPR profiles, CO-FTIR spectra and XPS spectra of NixFey/SiO2 catalysts and (b) adsorption configurations of acetic acid, H, OH on clean surfaces and potential diagrams of acetic acid deoxidation on Ni(111) surface[83]

图8. (a) 新鲜和使用后的Pt/γ-Al2O3催化剂的HAADF-STEM图像、H2-TPR图像、m/z=18的质量碎片的程序升温脱附(TPD)图谱、BJH方法计算的孔径分布(BJH PSD)曲线和吡啶化学吸附傅里叶变换红外光谱[96]和(b) Fe-N-C@Al2O3催化剂的XRD图谱、拉曼光谱和Al2O3和TiO2载体的吡啶化学吸附傅里叶变换红外光谱[100]

Figure 8. HAADF-STEM image, H2-TPR profile, profiles of the mass fragment m/z=18 in TPD experiments, BJH PSD curves and pyridine-chemisorbed FT-IR spectra of the fresh and spent Pt/γ-Al2O3 catalysts[96] and (b) XRD patterns and Raman spectra of Fe-N-C@Al2O3 catalysts, IR spectra of pyridine adsorbed on Al2O3 and TiO2 support[100]

图9. (a) Ni/Al-SBA-15催化剂的XRD图谱、HRTEM图像、吡啶化学吸附的漫反射傅里叶变换红外光谱以及在辛酸转化率为13%~20%时, 产物选择性与催化剂酸性位数量的关系[105]和(b) Ni/HUSY催化剂的N2吸脱附等温线、BJH吸附孔径分布、27Al MAS NMR和29Si MAS NMR光谱以及HAADF-STEM和HRTEM图像[110]

Figure 9. (a) XRD patterns, HRTEM image, DRIFT spectra of chemisorbed pyridine of Ni/Al-SBA-15 catalysts and product selectivity at 13%~20% isoconversion over Ni/Al-SBA-15 catalysts as a function of acid site loading[105] and (b) N2 adsorption and desorption isotherms, BJH adsorption pore size distribution, 27Al MAS NMR and 29Si MAS NMR spectra, HAADF-STEM and TEM measurements of Ni/HUSY catalysts[110]

图10. (a) NixWy/SiO2催化剂合成示意图、XRD图谱、HAADF-STEM图像、HRTEM图像、金属颗粒分布统计(PSD)图、Ni7W3/SiO2中W的4f轨道的XPS光谱图、催化剂氧空位比值与烷烃产率的关系曲线以及丙酸和H在Ni(111)、W2O5/Ni(111)-Ni、W2O5/Ni(111)-OV、W2O6/Ni(111)-Ni表面的吸附构型[129]、(b) Ni-MoS2催化剂在H2气氛下催化脂肪酸脱羧的反应机理示意图[57]和(c)不同浓度油酸铁毒化的MoS2/γ-Al2O3催化剂在油酸加氢脱氧过程中对不同产物选择性的时间曲线、毒化和未毒化的催化剂使用后的H2-TPR图像、毒化催化剂使用后的HAADF-STEM和EDX mapping图像[133]

Figure 10. (a) Synthesis approach illustration, XRD patterns, HAADF-STEM, HRTEM, PSD image of NixWy/SiO2 catalysts and XPS analysis of W 4f in Ni7W3/SiO2 catalysts, the relationship between OV ratios and C17+C18 yield, the optimized configurations of propionic acid and H adsorption on surfaces of Ni(111), W2O5/Ni(111)-Ni, W2O5/Ni(111)-OV and W2O6/Ni(111)-Ni[129], (b) suggested mechanism for the decarbonylation of fatty acids on Ni-MoS2 catalyst under an H2 atmosphere[57] and (c) selectivity of major products during hydrodeoxygenation of oleic acid over MoS2/γ-Al2O3 with varying concentrations of Fe-oleate poisoned, H2-TPR profiles of recovered poisoned and unpoisoned catalysts, HAADF-STEM and corresponding EDX mapping of recovered poisoned catalysts[133]

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第二代生物柴油制备的多相催化剂的结构设计及研究进展

Structural Design and Research Progress of Heterogeneous Catalysts for the Preparation of Second Generation Biodiesel

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