1. State Key Laboratory of Heavy Oil Processing, China University of Petroleum, Qingdao 266580, China 2. SINOPEC (Dalian) Research Institute of Petroleum and Petrochemical Co., Ltd., Dalian 116000, China
Similar to Sn, Pb located at the same group (IVA) in the periodic table of elements, can also catalyze propane dehydrogenation to propene, while a fast deactivation can be observed. To enhance the stability, the traditional carrier Al2O3 with a small amount, was introduced into Pb/SiO2 catalyst in this study. It has been proved that Al2O3 can inhibit the reduction of PbO, and weaken the agglomeration and loss of Pb species due to its enhanced interaction with Pb species. As a result, 3Al15Pb/SiO2 catalyst exhibits a much higher stability up to more than 150 h. In addition, a simple schematic diagram of the change of surface species on the catalyst surface after Al2O3 addition was also proposed.
G W Wang, H L Zhang, H R Wang, Q Q Zhu, C Y Li, H H Shan. The role of metallic Sn species in catalytic dehydrogenation of propane: active component rather than only promoter. Journal of Catalysis, 2016, 344: 606–608 https://doi.org/10.1016/j.jcat.2016.11.003
2
G W Wang, H L Zhang, Q Q Zhu, Z X Lin, X Y Li, H Wang, C Y Li, H H Shan. Sn-containing hexagonal mesoporous silica (HMS) for catalytic dehydrogenation of propane: an efficient strategy to enhance stability. Journal of Catalysis, 2017, 351: 90–94 https://doi.org/10.1016/j.jcat.2017.04.018
3
H R Wang, H Wang, X Y Li, C Y Li. Nature of active tin species and promoting effect of nickle in silica supported tin oxide for dehydrogenation of propane. Applied Surface Science, 2017, 407: 456–462 https://doi.org/10.1016/j.apsusc.2017.02.216
4
H R Wang, H W Huang, K Bashir, C Y Li. Isolated Sn on mesoporous silica as a highly stable and selective catalyst for the propane dehydrogenation. Applied Catalysis A: General, 2020, 590: 117291–117298 https://doi.org/10.1016/j.apcata.2019.117291
5
H Zhang, Y Jiang, W Dai, N Tang, X Zhu, C Li, H Shan, G Wang. Catalytic dehydrogenation of propane over unconventional Pb/SiO2 catalysts. Fuel, 2022, 318: 123532–123537 https://doi.org/10.1016/j.fuel.2022.123532
6
X Y Zhu, T H Wang, Z K Xu, Y Y Yue, M G Lin, H B Zhu. Pt–Sn clusters anchored at Al3+penta sites as a sinter-resistant and regenerable catalyst for propane dehydrogenation. Journal of Energy Chemistry, 2022, 65: 293–301 https://doi.org/10.1016/j.jechem.2021.06.002
7
Y H Dai, J J Gu, S Y Tian, Y Wu, J C Chen, F X Li, Y H Du, L M Peng, W P Ding, Y H Yang. γ-Al2O3 sheet-stabilized isolate Co2+ for catalytic propane dehydrogenation. Journal of Catalysis, 2020, 381: 482–492 https://doi.org/10.1016/j.jcat.2019.11.026
8
M Arora, S Baccaro, G Sharma, D Singh, K S Thind, D P Singh. Radiation effects on PbO-Al2O3-B2O3-SiO2 glasses by FTIR spectroscopy. Nuclear Instruments & Methods in Physics Research, 2009, 267(5): 817–820 https://doi.org/10.1016/j.nimb.2009.01.003
9
M Leśniak, J Partyka, K Pasiut, M Sitarz. Microstructure study of opaque glazes from SiO2-Al2O3-MgO-K2O-Na2O system by variable molar ratio of SiO2/Al2O3 by FTIR and Raman spectroscopy. Journal of Molecular Structure, 2016, 1126: 240–250 https://doi.org/10.1016/j.molstruc.2015.12.072
10
C H Li, P Sengodu, D Y Wang, T R Kuo, C C Chen. Highly stable cycling of a lead oxide/copper nanocomposite as an anode material in lithium ion batteries. RSC Advances, 2015, 5(62): 50245–50252 https://doi.org/10.1039/C5RA07948A
11
Y B Saddeek, M S Gaafar, S A Bashier. Structural influence of PbO by means of FTIR and acoustics on calcium alumino-borosilicate glass system. Journal of Non-Crystalline Solids, 2010, 356(20–22): 1089–1095 https://doi.org/10.1016/j.jnoncrysol.2010.01.010
12
M Nafees, M Ikram, S Ali. Thermal stability of lead sulfide and lead oxide nano-crystalline materials. Applied Nanoscience, 2017, 7(7): 399–406 https://doi.org/10.1007/s13204-017-0578-7
13
P H Zhang, Y N Wang, Y M Sui, C Z Wang, B B Liu, G T Zou, B Zou. A facile method to synthesize nanosized metal oxides from their corresponding bulk materials. CrystEngComm, 2012, 14(18): 5937–5942 https://doi.org/10.1039/c2ce25398d
14
S K Noukelag, H E A Mohamed, L C Razanamahandry, S K O Ntwampe, C J Arendse. Bio-inspired synthesis of PbO nanoparticles (NPs) via an aqueous extract of Rosmarinus officinalis (rosemary) leaves. Materials Today: Proceedings, 2021, 36: 421–426 https://doi.org/10.1016/j.matpr.2020.04.852
15
A Dandapat, D Jana, G De. Synthesis of thick mesoporous gamma-alumina films, loading of Pt nanoparticles, and use of the composite film as a reusable catalyst. ACS Applied Materials & Interfaces, 2009, 1(4): 833–840 https://doi.org/10.1021/am800241x
16
J H Kwak, J Hu, D Mei, C W Yi, D H Kim, C H F Peden, L F Allard, J Szanyi. Coordinatively unsaturated Al3+ centers as binding sites for active catalyst phases of platinum on gamma-Al2O3. Science, 2009, 325(5948): 1670–1673 https://doi.org/10.1126/science.1176745
17
L Shi, G M Deng, W C Li, S Miao, Q N Wang, W P Zhang, A H Lu. Al2O3 nanosheets rich in pentacoordinate Al3+ ions stabilize Pt–Sn clusters for propane dehydrogenation. Angewandte Chemie International Edition, 2015, 54(47): 13994–13998 https://doi.org/10.1002/anie.201507119
18
N F Tang, Y Cong, Q Shang, C Wu, G Xu, X Wang. Coordinatively unsaturated Al3+ sites anchored subnanometric ruthenium catalyst for hydrogenation of aromatics. ACS Catalysis, 2017, 7(9): 5987–5991 https://doi.org/10.1021/acscatal.7b01816
19
M Mudgal, A Singh, R K Chouhan, A Acharya, A K Srivastava. Fly ash red mud geopolymer with improved mechanical strength. Cleaner Engineering and Technology, 2021, 4: 100215–100221 https://doi.org/10.1016/j.clet.2021.100215
20
M Kanuchova, L Kozakova, M Drabova, M Sisol, A Estokova, J Kanuch, J Skvarla. Monitoring and characterization of creation of geopolymers prepared from fly ash and metakaolin by X-ray photoelectron spectroscopy method. Environmental Progress & Sustainable Energy, 2015, 34(3): 841–849 https://doi.org/10.1002/ep.12068
21
J Kwak, J Hu, D Kim, J Szanyi, C Peden. Penta-coordinated Al3+ ions as preferential nucleation sites for BaO on γ-Al2O3: an ultra-high-magnetic field 27Al MAS NMR study. Journal of Catalysis, 2007, 251(1): 189–194 https://doi.org/10.1016/j.jcat.2007.06.029
22
L A O’Dell, S L P Savin, A V Chadwick, M E A Smith. 27Al MAS NMR study of a sol–gel produced alumina identification of the NMR parameters of the θ-Al2O3 transition alumina phase. Solid State Nuclear Magnetic Resonance, 2007, 31(4): 169–173 https://doi.org/10.1016/j.ssnmr.2007.05.002
23
S N Dong, W J Shi, J Zhang, S P Bi. 27Al NMR chemical shifts and relative stabilities of aqueous monomeric Al3+ hydrolytic species with different coordination structures. ACS Earth & Space Chemistry, 2019, 3(7): 1353–1361 https://doi.org/10.1021/acsearthspacechem.9b00102
24
G Wendt, C D Meinecke, W Schmitz. Oxidative dimerization of methane on lead oxide-alumina catalysts. Applied Catalysis, 1988, 45(2): 209–220 https://doi.org/10.1016/S0166-9834(00)83030-4
25
S L Wang, H Y Niu, J J Wang, T Chen, G Y Wang, J M Zhang. Highly effective transformation of methyl phenyl carbonate to diphenyl carbonate with recyclable Pb nanocatalyst. RSC Advances, 2019, 9(35): 20415–20423 https://doi.org/10.1039/C9RA03931G
