调控等级孔UiO-66(Ce)中Ru纳米团簇的电子态、丰度和微环境用于高效催化双环戊二烯加氢

doi:10.1016/S1872-2067(23)64562-0

催化学报 ›› 2024, Vol. 56: 150-165.DOI: 10.1016/S1872-2067(23)64562-0

调控等级孔UiO-66(Ce)中Ru纳米团簇的电子态、丰度和微环境用于高效催化双环戊二烯加氢

李如硕^a^,¹, 汪琳梦^a^,¹, 周佩云^a, 林璟^a, 刘志远^a, 陈娟^a, 赵丹凤^a, 黄秀兵^a^,^*(), 陶志平^b^,^*(), 王戈^a^,^*()

^a北京科技大学材料科学与工程学院, 北京基因组工程材料高级创新中心, 北京分子与结构构建功能材料重点实验室, 北京100083
^b中国石化石油化工科学研究院有限公司, 北京100083

收稿日期:2023-09-13 接受日期:2023-11-10 出版日期:2024-01-18 发布日期:2024-01-10
通讯作者: *电子信箱: xiubinghuang@ustb.edu.cn (黄秀兵), taozhiping.ripp@sinopec.com (陶志平), gewang@ustb.edu.cn (王戈).
作者简介:¹共同第一作者.
基金资助:
国家重点研发计划(2021YFB3500700);国家自然科学基金(51972024);广东省自然科学基金(2022A1515010185)

Electronic state, abundance and microenvironment modulation of Ru nanoclusters within hierarchically porous UiO-66(Ce) for efficient hydrogenation of dicyclopentadiene

Rushuo Li^a^,¹, Linmeng Wang^a^,¹, Peiyun Zhou^a, Jing Lin^a, Zhiyuan Liu^a, Juan Chen^a, Danfeng Zhao^a, Xiubing Huang^a^,^*(), Zhiping Tao^b^,^*(), Ge Wang^a^,^*()

^aBeijing Advanced Innovation Center for Materials Genome Engineering, Beijing Key Laboratory of Function Materials for Molecule & Structure Construction, School of Materials Science and Engineering, University of Science and Technology Beijing, Beijing 100083, China
^bSinopec Research Institute of Petroleum Processing Co., Ltd., Beijing 100083, China

Received:2023-09-13 Accepted:2023-11-10 Online:2024-01-18 Published:2024-01-10
Contact: *E-mail: xiubinghuang@ustb.edu.cn (X. Huang), taozhiping.ripp@sinopec.com (Z. Tao), gewang@ustb.edu.cn (G. Wang).
About author:¹Contributed equally to this work.
Supported by:
National Key Research and Development Program of China(2021YFB3500700);National Natural Science Foundation of China(51972024);Natural Science Foundation of Guangdong Province(2022A1515010185)

摘要/Abstract

摘要：

催化石油加工副产物双环戊二烯(DCPD)加氢得到的四氢双环戊二烯(THDCPD)是一种高能量密度燃料, 在航空航天领域具有重要应用价值. 传统DCPD加氢催化剂在反应中存在使用寿命短和重复使用性差等问题. 金属有机框架(MOFs)作为一种周期有序多孔材料, 有望成为用于DCPD加氢的新型高效催化剂. 通过引入介孔或大孔来构建等级孔MOFs (HP-MOFs), 可以克服微孔对DCPD等大客体分子的扩散限制, 促进底物分子向HP-MOFs内部活性位点转移. 此外, 加入合适的金属组分(如价格相对低廉的Ru)到HP-MOFs, 可以使金属的原子利用率最大化, 优化活性位点的分散性和稳定性, 进一步协同提升催化性能. 因此, 发展HP-MOFs与金属组分间异质结构的调控方法, 建立构效关系至关重要.

本文采用软模板法制备了HP-UiO-66(Ce), 设计和构建了介孔UiO-66(Ce)负载钌纳米簇(NCs)异质材料, 并用于催化DCPD加氢反应. X射线衍射(XRD)、扫描电镜、透射电镜、氮气吸脱附和DCPD加氢结果表明, 与微孔和大孔UiO-66(Ce)相比, 介孔UiO-66(Ce)独特的结构在催化剂制备和DCPD加氢中显示出独特的优势: (1)具有配体缺失缺陷的Ce-oxo簇促进了Ru³⁺的有效吸附; (2) 微孔框架的约束作用实现了Ru NCs的有效固定和均匀分散, 抑制了Ru NCs的团聚和流失, 保证了催化剂的稳定性; (3) 介孔结构为DCPD和H₂底物分子提供了高效的传质通道, 也有利于暴露更多的活性中心, 促进DCPD与H₂底物分子的吸附和活化. 此外, 通过优化合成条件, 可以精确控制Ru NCs活性位点的电子结构、分布和微环境. XRD和X射线光电子能谱结果表明, Ru NCs和Meso-UiO-66(Ce)之间Ru-O-Ce强异质界面的形成导致了晶格畸变, Ru@Meso-UiO-25-200中Ru⁰和M-O占比最多, 主要来源于还原处理得到的Ru NCs和Ru-O-Ce异质界面中Ru‒O键的形成, 且样品中Ru⁰的含量与Ru³⁺吸附温度呈反相关趋势, 与样品还原温度呈正相关趋势. 密度泛函理论计算结果表明, 金属Ru⁰作为主要活性位点, 极大地促进了DCPD和H₂的吸附, 并激活了催化剂上吸附的DCPD的C=C键, 促进了DCPD两个C=C双键的“共吸附”和连续化加氢过程. 因此, 介孔UiO-66(Ce)和Ru NCs异质结构的构建, 在低温(60 °C)下仅用35 min就实现了DCPD催化加氢得到四氢双环戊二烯(THDCPD)(100%转化率和~100%选择性), 且循环使用6次后性能基本保持不变, 表现出较好的活性和稳定性.

综上, 本文通过等级孔和异质结构的构筑, 证明了介孔结构在大底物分子催化反应中的结构优越性, 并进一步揭示了催化剂合成条件、结构和性能之间的关系, 为理性设计新型MOFs基功能材料在催化、吸附、储能等方面的应用提供新思路.

关键词: 等级孔, UiO-66(Ce), Ru纳米簇, 双环戊二烯, 微环境调控

Abstract:

Developing catalysts for dicyclopentadiene (DCPD) hydrogenation to tetrahydrodicyclopentadiene (THDCPD) at low temperature is crucial and challenging for the green and energy-saving production of high energy density aviation fuel. Herein, hierarchically porous UiO-66(Ce) encapsulate Ru nanoclusters (NCs) was successfully customized by soft template method and in-situ reduction. The mesoporous UiO-66(Ce) promoted the high dispersion of Ru NCs, and the transfer of substrate molecules. By controlling the synthesis conditions, the electronic state, abundance, and microenvironment of Ru NCs were precisely regulated. Theory calculation and experimental results revealed that metallic Ru as the main active sites greatly promoted the adsorption and activation of substrate molecules. Therefore, mesoporous UiO-66(Ce) encapsulated Ru NCs showed remarkable catalytic DCPD hydrogenation performance with DCPD conversion of 100% and THDCPD selectivity of ~100% (60 °C, only 35 min). This study has brought new inspiration and guidance to the rational design of function materials for various catalytic applications.

Key words: Hierarchically porous, UiO-66(Ce), Ru nanoclusters, Dicyclopentadiene, Microenvironment modulation

李如硕, 汪琳梦, 周佩云, 林璟, 刘志远, 陈娟, 赵丹凤, 黄秀兵, 陶志平, 王戈. 调控等级孔UiO-66(Ce)中Ru纳米团簇的电子态、丰度和微环境用于高效催化双环戊二烯加氢[J]. 催化学报, 2024, 56: 150-165.

Rushuo Li, Linmeng Wang, Peiyun Zhou, Jing Lin, Zhiyuan Liu, Juan Chen, Danfeng Zhao, Xiubing Huang, Zhiping Tao, Ge Wang. Electronic state, abundance and microenvironment modulation of Ru nanoclusters within hierarchically porous UiO-66(Ce) for efficient hydrogenation of dicyclopentadiene[J]. Chinese Journal of Catalysis, 2024, 56: 150-165.

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图/表 11

Scheme 1. Schematic illustration of the HP-UiO-66(Ce) encapsulated Ru NCs.

Fig. 1. High-magnification SEM images of Micro-UiO-66 (a), Meso-UiO-66 (b) and Macro-UiO-66 (d). (c) TEM image of Meso-UiO-66. Nitrogen sorption isotherms (e) and corresponding pore size distributions (f) (calculated by DFT-analysis) for the Micro-UiO-66 and Meso-UiO-66.

Fig. 2. High-magnification SEM images of Ru@Meso-UiO-25-200 (a), Ru@Micro-UiO-25-200 (b), and Ru@Macro-UiO-25-200 (c). The low-magnification (d) and high-magnification (e,f) TEM images, and HAADF-STEM image (g) with elemental mapping images of Ru@Meso- UiO-25-200.

Fig. 3. XPS full survey (a), Ru 3p (b), Ce 3d (c), O 1s (d) spectra, and structure schematic illustration (e) of Ru3+-Meso-UiO-25, Ru@Meso-UiO-25-150, Ru@Meso-UiO-25-180, and Ru@Meso-UiO-25-200.

Fig. 4. Powder XRD patterns of HP-UiO-66(Ce) with different pore sizes encapsulated Ru NCs (a), Meso-UiO-66 reduced at different temperatures (b), Meso-UiO-66 encapsulated Ru NCs reduced at different temperatures (c), Meso-UiO-66 encapsulated Ru NCs with different Ru loadings (d), Meso-UiO-66 with different Ru3+ adsorption temperatures (e), and Meso-UiO-66 encapsulated Ru NCs with different Ru3+ adsorption temperatures (f).

Fig. 5. TEM, HRTEM, and Ru NCs size distribution images of Ru@Meso-UiO-25-200 (a-c), Ru@Meso-UiO-30-200 (d-f), Ru@Meso- UiO-35-200 (g-i), Ru@Meso-UiO-40-200 (j-l), and Ru@Meso-UiO- 60-200 (m-o).

Table 1 Catalytic performances towards the hydrogenation of DCPD over different catalysts for comparison a.

Entry	Sample	T (°C)	t (h)	Con. ^b(%)	Sel. ^c (%)
Entry	Sample	T (°C)	t (h)	DCPD	DHDCPD	THDCPD
1	Micro-UiO-66	100	10	5	100	—
2	Macro-UiO-66	100	5	6.7	100	—
3	Meso-UiO-66	100	5	13.2	100	—
3	Meso-UiO-66	—	2	0	—	—
4	Meso-UiO-200	100	2	6.4	100	—
5	Ru@Micro-UiO-25-200	60	1	5.4	77.3	22.7
6	Ru@Macro-UiO-25-200	60	0.5	38.8	9.3	90.7
7	Ru@Meso-UiO-25-200	60	0.5	99.7	9.1	90.9
8	Ru@Meso-UiO-25-180	60	1	0	—	—
9	Ru@Meso-UiO-25-150	60	1	0	—	—
10	1.5Ru@Meso-UiO-25-200	60	0.5	7	42.7	57.3
11	1Ru@Meso-UiO-25-200	60	0.5	0	—	—
12	0.5Ru@Meso-UiO-25-200	60	0.5	0	—	—
13	Ru@Meso-UiO-30-200	60	0.5	78.7	27.8	72.1
14	Ru@Meso-UiO-35-200	60	0.5	3.8	69.2	30.8
15	Ru@Meso-UiO-40-200	60	0.5	0.8	56	44
16	Ru@Meso-UiO-60-200	60	0.5	0	—	—

Fig. 6. Conversion of DCPD (a) and selectivity of DHDCPD and THDCPD (b) over Ru@Meso-UiO-25-200 at different reaction times. (c,d) Reusability of Ru@Meso-UiO-25-200-AF-H2/Ar in the hydrogenation reaction of DCPD (t = 35 min). Reaction conditions: mDCPD = 200 mg, mcatalyst = 20 mg, Vsolvent = 5 mL, PH2 = 2 MPa, T = 60 °C.

Fig. 7. The optimized simplified structures of Meso-UiO-66 (a), and Ru@Meso-UiO-25-200 (b). (c) The adsorption energy of H2 and DCPD chemisorbed and physiosorbed on Meso-UiO-66 and Ru@Meso- UiO-25-200, ** and * represent physisorbed and chemisorbed species respectively. The structures of catalysts, H2 and DCPD are displayed as ball-and-stick models in which yellow, green, gray, white, and red balls represent Ce, Ru, C, H and O, respectively.

Fig. 8. PDOS of DCPD and H2 adsorbed on Ru@Meso-UiO-25-200 (a,b) and Meso-UiO-66 (c,d), respectively. The Fermi level is set to zero as shown as dashed line. The optimized models of chemisorbed H2 (e) and physisorbed DCPD (f) on Ce-O sites of Meso-UiO-66, chemisorbed H2 (g) and chemisorbed DCPD (h) on Ru active sites of Ru@Meso-UiO-25-200. Charge density difference for DCPD and H2 adsorbed on Ru@Meso-UiO-25-200 (i,j) and Meso-UiO-66 (k,l), respectively. Red and blue represent electron accumulation and depletion, and the isosurface value is set as 0.005 a.u. Charge transfer (ΔQ, e) are calculated from the population analysis in Hirshfeld method.

Fig. 9. Possible reaction pathways of DCPD hydrogenation over the Ru@Meso-UiO-25-200.

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调控等级孔UiO-66(Ce)中Ru纳米团簇的电子态、丰度和微环境用于高效催化双环戊二烯加氢

Electronic state, abundance and microenvironment modulation of Ru nanoclusters within hierarchically porous UiO-66(Ce) for efficient hydrogenation of dicyclopentadiene

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