TeOx改性MoVTeNbO表面工程促进甲苯同系物氧化为醛

doi:10.1016/S1872-2067(24)60137-3

催化学报 ›› 2024, Vol. 66: 268-281.DOI: 10.1016/S1872-2067(24)60137-3

TeO_x改性MoVTeNbO表面工程促进甲苯同系物氧化为醛

邓长顺^a^,¹, 葛冰青^a^,¹, 姚均^a, 赵涛涛^a, 沈辰阳^a, 张哲玮^a, 王涛^b, 郭向可^a, 薛念华^a, 郭学锋^a, 彭路明^a, 祝艳^a, 丁维平^a^,^*()

^a南京大学化学化工学院, 介观化学教育部重点实验室, 江苏南京 210023
^b江苏介观催化材料科技有限公司, 江苏苏州 215634

收稿日期:2024-07-27 接受日期:2024-09-04 出版日期:2024-11-18 发布日期:2024-11-10
通讯作者: *电子邮箱: dingwp@nju.edu.cn (丁维平).
作者简介:¹共同第一作者.
基金资助:
国家自然科学基金(22202101);国家自然科学基金(21932004);国家自然科学基金(91963206);国家自然科学基金(22172072);国家重点研发计划(2021YFA1500301);江苏省自然科学基金(BK20231401);国家资助博士后研究人员计划(GZC20231102)

Surface engineering of TeO_x modification on MoVTeNbO creates a high-performance catalyst for oxidation of toluene homologues to aldehydes

Changshun Deng^a^,¹, Bingqing Ge^a^,¹, Jun Yao^a, Taotao Zhao^a, Chenyang Shen^a, Zhewei Zhang^a, Tao Wang^b, Xiangke Guo^a, Nianhua Xue^a, Xuefeng Guo^a, Luming Peng^a, Yan Zhu^a, Weiping Ding^a^,^*()

^aKey Laboratory of Mesoscopic Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, Jiangsu, China
^bJiangsu Meso Catalytic Materials Technology Co., Ltd, Suzhou 215634, Jiangsu, China

Received:2024-07-27 Accepted:2024-09-04 Online:2024-11-18 Published:2024-11-10
Contact: *E-mail: dingwp@nju.edu.cn (W. Ding).
About author:¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22202101);National Natural Science Foundation of China(21932004);National Natural Science Foundation of China(91963206);National Natural Science Foundation of China(22172072);Ministry of Science and Technology of China(2021YFA1500301);Jiangsu Provincial Natural Science Foundation of China(BK20231401);Postdoctoral Fellowship Program of CPSF(GZC20231102)

摘要/Abstract

摘要：

烃类分子选择氧化生成有机含氧产物是一类极其重要的反应, 其将氧原子引入碳氢化合物中, 能产生用途广泛且价值更高的化学品. 作为最简单的芳香醛, 苯甲醛是非常重要的精细化学品和有机合成中间体, 广泛应用于香料、食品和医药等行业. 当前生产苯甲醛的工业过程主要有甲苯氯化水解法和甲苯均相氧化法, 但均存在严重的设备腐蚀和环境污染问题, 且生产的苯甲醛常含有微量卤素, 阻碍了其在医药和食品等领域的应用. 无卤素和自由基引发剂条件下催化甲苯分子氧氧化制苯甲醛在绿色化学研究中极具挑战. 因此, 开发常压下高效、高选择性的催化剂和绿色工艺具有重要的科学意义和工业价值.

本文报道了一种表面工程的策略, 通过TeO_x改性MoVTeNbO, 综合考虑活性、选择性和稳定性, 制得的TeO_x/MoVTeNbO催化剂具有较好的甲苯分子氧绿色氧化制苯甲醛性能. 首先, 理论研究发现, 在MoVTeNbO表面的V=O活性中心周围构筑适量离散型TeO_x团簇, 屏蔽了与甲苯分子苯环强烈相互作用的非选择性氧化位点, 使甲苯分子垂直化学吸附在其表面, 甲苯甲基在重构的选择性氧化位点上易于氧化为苯甲醛, 其中V=O负责从甲基中连续提取氢并植入氧以形成苯甲醛, TeO_x团簇通过可变化合价参与该反应并通过与苯甲醛的-CHO基团偶联作用稳定苯甲醛, 从而实现其高选择性. X射线衍射、高分辨透射电镜和能谱仪结果表明, TeO_x高分散于MoVTeNbO表面. 拉曼光谱、傅里叶变换红外光谱、电子顺磁共振谱、X射线光电子能谱及同步辐射X射线吸收谱等结果表明, TeO_x主要以离散型团簇形式聚集于V=O活性中心周围, 与V=O活性中心存在强烈相互作用并形成了新的Te-O-V键. 催化性能评价和动力学结果表明, MoVTeNbO表面构筑的适量TeO_x团簇显著抑制了苯甲醛过度氧化和甲苯燃烧反应, 最佳条件下实现甲苯转化率高达~24%, 苯甲醛选择性>95%, 且催化剂具有较好的稳定性. 原位红外光谱和X射线光电子能谱结果表明, MoVTeNbO表面构筑TeO_x团簇使得甲苯在催化剂表面由平躺吸附(MoVTeNbO)转变为甲基朝下的垂直吸附(TeO_x/MoVTeNbO), 主要产物也由马来酸酐转变为苯甲醛, 且V=O活性中心与其周围的TeO_x团簇均参与了甲苯活化和氧化. 值得注意的是, 上述新的反应机理同样适用于甲苯同系物选择氧化为醛, 且催化剂表现出高选择性和活性, 其中对氯甲苯氧化为对氯苯甲醛选择性>99%, 转化率>28%.

综上, 本文提出了TeO_x改性的MoVTeNbO表面工程策略, 用于合成TeO_x团簇离散沉积于表面的TeO_x/MoVTeNbO催化剂, 实现常压固定床反应器中甲苯同系物分子氧到醛的高选择性氧化. 该方法的关键是离散型TeO_x团簇沉积在MoVTeNbO表面并围绕V=O活性位点, 甲苯在催化剂重排后的表面上的吸附构型从平躺吸附变为甲基朝下的垂直吸附, 从而实现甲苯高选择氧化为苯甲醛. 该工作丰富和深化了对典型催化氧化过程的认识, 为烃类绿色氧化制含氧产物高效催化剂设计提供了新的思路.

关键词: 表面工程, TeO_x/MoVTeNbO, 甲苯氧化, 苯甲醛, 分子氧

Abstract:

The heterogeneous catalytic oxidation of toluene by O₂ is an inherently safe and green route for production of benzaldehyde, but after more than fifty years of effort, it remains a great challenge. Here, we report the best heterogeneous catalyst, TeO_x/MoVTeNbO, up to now for the green oxidation of toluene by O₂ to benzaldehyde, balancing the catalyst activity, selectivity, and stability. The deposition of TeO_x endows the MoVTeNbO composite oxide with entirely new property for toluene oxidation and the surface engineering mechanism has been fully explained. The discrete TeO_x clusters on the surface, shielding the nonselective oxidation sites that interact strongly with the benzene ring of toluene molecule, allows toluene molecule to chemically adsorb to the surface perpendicularly and the methyl is then prone to oxidation to aldehyde on the reshaped selective oxidation sites, where V=O is the main active species responsible for continuously extracting hydrogen from methyl and implanting oxygen to form benzaldehyde. The TeO_x clusters participate in this reaction through variable valences and stabilize benzaldehyde by couple interaction with the -CHO group of benzaldehyde, thereby achieving high selectivity to benzaldehyde (>95%). The extended works indicate that the catalytic mechanism is effective in a series of selective oxidation of toluene homologues to corresponding aldehydes.

Key words: Surface engineering, TeO_x/MoVTeNbO, Toluene oxidation, Benzaldehyde, Molecular oxygen

邓长顺, 葛冰青, 姚均, 赵涛涛, 沈辰阳, 张哲玮, 王涛, 郭向可, 薛念华, 郭学锋, 彭路明, 祝艳, 丁维平. TeO_x改性MoVTeNbO表面工程促进甲苯同系物氧化为醛[J]. 催化学报, 2024, 66: 268-281.

Changshun Deng, Bingqing Ge, Jun Yao, Taotao Zhao, Chenyang Shen, Zhewei Zhang, Tao Wang, Xiangke Guo, Nianhua Xue, Xuefeng Guo, Luming Peng, Yan Zhu, Weiping Ding. Surface engineering of TeO_x modification on MoVTeNbO creates a high-performance catalyst for oxidation of toluene homologues to aldehydes[J]. Chinese Journal of Catalysis, 2024, 66: 268-281.

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图/表 8

Scheme 1. (a) Traditional routes used in current industry. (b) Direct oxidation of toluene to benzaldehyde or homologues by O2 in this work.

Fig. 1. (a) Atomic (001) surface model of the M1 phase MoVTeNbO complex oxides and the ODH reaction ODH of ethane to ethene. (b) V=O active site on the (001) plane of M1 phase and the oxidation of propane to acrylic acid. (c) Atomic (001) surface model of the M1 phase and the oxidation of toluene to maleic anhydride. (d) TeOx/MVTN with TeOx clusters on (001) surface of the M1 phase MoVTeNbO complex oxides in suitable density and self-organized structure presented in this work, for toluene oxidation by O2 to benzaldehyde.

Fig. 2. (a) Configuration of toluene adsorption (inset) and corresponding energy with the density of TeOx on MVTN. (b-d) Atomic models about toluene reaction to benzaldehyde over MVTN (b) and TeOx/MVTN (d), with intermediates and transition states, corresponding to the energy steps diagram (c). Atomic models about the reaction of benzaldehyde to benzoic acid over MVTN (e) and TeOx/MVTN (g), with the corresponding energy steps diagram (f). The reactive area of MVTN and TeOx/MVTN involved the V=O active site containing the pentameric ensembles (S4)2-S2-(S7)2.

Fig. 3. HRTEM images of MVTN (a) and TeOx/MVTN (b). Raman (c), FT-IR (d), EPR (e), and V 2p (f) XPS spectra of MVTN and TeOx/MVTN. Vanadium k-edge XAS spectra (V foil, VO2, and V2O5 were used as references). Normalized XANES (g), Radial distribution function from EXAFS (h), and wavelet transform maps (i) of Fourier transformed k2-weighted χ(k). (j-l) Tellurium k-edge XAS spectra (Te foil, TeO2, and H6TeO6 were used as references). Normalized XANES (j), EXAFS (k), and wavelet transform maps (l) of Fourier transformed k2-weighted χ(k).

Fig. 4. (a) Catalytic performance for toluene reaction over MVTN and TeOx/MVTN (toluene: 0.6 μL·min?1, vaporized in the line; O2: 5 mL·min?1; N2: 20 mL·min?1; cat.: 0.3 g; 400 °C). (b) Effect of TeOx loading on product selectivity (toluene: 1 μL·min?1, vaporized in the line; O2: 5 mL·min?1; N2: 20 mL·min?1; cat.: 0.3 g; 400 °C). (c) Effect of molar ratio of O2 to toluene on the catalytic performance over TeOx/MVTN (toluene: 0.6 μL·min?1, vaporized in the line; O2: 2-6 mL·min?1; N2: 19-23 mL·min?1; cat.: 0.3 g; 400 °C). (d) Effect of the WHSV on the catalytic performance over TeOx/MVTN (toluene: 0.6 μL·min?1, vaporized in the line; O2: 5 mL·min?1; N2: 0-30 mL·min?1; cat.: 0.3 g; 400 °C). (e) Prolonged reaction of TeOx/MVTN (toluene: 1 μL·min?1, vaporized in the line; O2: 5 mL·min?1; N2: 20 mL·min?1; cat.: 0.3 g; 350 °C). Arrhenius plots (f), dependences of the reaction rate on the partial pressure of toluene (g) and O2 (h) over MVTN and TeOx/MVTN (toluene: 0.2-1.6 μL·min?1, vaporized in the line; O2: 1-7 mL·min?1; balance N2; total flow rate: 25 mL·min?1; cat.: 0.3 g; 250-400 °C). MD simulation (MSD) of toluene (i) and O2 (j) molecules with different atomic concentrations on the surface of MVTN and TeOx/MVTN (toluene: 0.8%-4%; O2: 9.6%-24%). Dependences of toluene and O2 diffusion coefficients obtained through MSD fitting on the concentration of toluene (k) and O2 (l).

Fig. 5. In-situ DRIFTS characterizations to capture the reaction intermediates over MVTN (a) and TeOx/MVTN (b) (toluene: 1 μL·min?1, vaporized in the line; O2: 5 mL·min?1; N2: 20 mL·min?1; cat.: 0.02 g; 350 °C for MVTN and 400 °C for TeOx/MVTN; time: 0-35 min). (c) Adsorption energy of carbon dioxide on MVTN and TeOx/MVTN, the inset shows the adsorption model of carbon dioxide on MVTN and TeOx/MVTN. (d) Te 3d XPS of TeOx/MVTN after use in toluene/O2 and toluene/Ar, respectively, at 400 °C.

Table 1 Toluene homologues reactions on TeOx/MVTN.

Entry	Conv. (%)	Product	Selec. (%)	Yield (%)
1	23.9		95.1	22.7
2	46.8		64.7	30.3
3	27.7		89.4	24.8
4	54.0		79.5	42.9
5^a	—	—	—	—
6^a	—	—	—	—
7	8.2		98.2	8.1
8	6.0		80.7	4.8
9	28.9		99.1	28.6
10^a	—	—	—	—
11	95.8		1.4	1.3

Fig. 6. Proposed reaction mechanism for p-chlorotoluene oxidation to p-chlorobenzaldehyde over TeOx/MVTN at the V=O active site located at the pentameric ensembles (S4)2-S2-(S7)2. The inset shows the calculated energy profiles in eV. The atomic configurations (side view) of the reaction intermediates of p-chlorotoluene oxidation to p-chlorobenzaldehyde are shown in the reaction cycle.

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TeO_x改性MoVTeNbO表面工程促进甲苯同系物氧化为醛

Surface engineering of TeO_x modification on MoVTeNbO creates a high-performance catalyst for oxidation of toluene homologues to aldehydes

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TeOx改性MoVTeNbO表面工程促进甲苯同系物氧化为醛

Surface engineering of TeOx modification on MoVTeNbO creates a high-performance catalyst for oxidation of toluene homologues to aldehydes

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TeO_x改性MoVTeNbO表面工程促进甲苯同系物氧化为醛

Surface engineering of TeO_x modification on MoVTeNbO creates a high-performance catalyst for oxidation of toluene homologues to aldehydes