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Selective Hydrogenation of Acetylene over Pd-In/Al2O3 Catalyst: Promotional Effect of Indium and Composition-dependent Performance Yueqiang Cao, Zhi Jun Sui, Yian Zhu, Xinggui Zhou, and De Chen ACS Catal., Just Accepted Manuscript • DOI: 10.1021/acscatal.7b01745 • Publication Date (Web): 10 Oct 2017 Downloaded from http://pubs.acs.org on October 10, 2017

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Selective Hydrogenation of Acetylene over PdIn/Al2O3 Catalyst: Promotional Effect of Indium and Composition-Dependent Performance Yueqiang Cao1, Zhijun Sui1, Yian Zhu1, Xinggui Zhou1,*, De Chen2,*

1 State Key Laboratory of Chemical Engineering, East China University of Science and Technology, 130 Meilong Road, Shanghai 200237, China

2 Department of Chemical Engineering, Norwegian University of Science and Technology, Trondheim 7491, Norway

*Corresponding author: Xinggui Zhou

Tel: +86-21-64253509; Fax: +86-21-64253528; Email: [email protected];

De Chen

Tel: +47-735-93149; Fax: +47-735-95047; Email: [email protected]

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Abstract: Highly dispersed bimetallic Pd-In catalysts on Al2O3 were prepared by simple impregnation method. Compared with the unsupported intermetallic catalyst, the supported Pd-In catalyst exhibited several magnitudes higher activity and similar selectivity for selective acetylene hydrogenation. Moreover, the activity, selectivity and anti-coking performance of the Pd-In catalyst was superior to those of the monometallic Pd catalyst. The electron transferred from indium weakened the adsorption of ethylene on the negatively charged Pd sites and hence improved the selectivity of Pd-In/Al2O3. The inhibited formation of hydride due to the presence of indium also contributed to the higher selectivity. The promoted activation of hydrogen, owing to the weak adsorption of acetylene on Pd-In/Al2O3, and decreased particle size jointly contributed to the enhanced activity of Pd-In/Al2O3. In addition, green oil formation on Pd-In/Al2O3 was retarded by the presence of indium, contributing to the enhanced stability of the catalyst. The bimetallic Pd-In catalysts showed a strongly composition-dependent performance, which is resulted from the different extent of electronic and/or geometric modification of Pd active sites.

Keywords: Acetylene hydrogenation; Pd/Al2O3; Hydride; Indium; Green oil


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1. Introduction Ethylene produced from the de-ethanizer unit steam-cracking process contains a small amount of acetylene which needs to be removed to avoid poisoning the downstream Ziegler-Natta catalyst for further polymerization.1-3 Hydrogenation of acetylene to ethylene is currently the most effective strategy to remove acetylene from ethylene and metal oxide supported Pd catalysts are commonly used for acetylene hydrogenation in industry. However, Pd catalysts usually exhibit limited selectivity and poor long-term stability, despite the high activity.4-6 The unsatisfactory selectivity of Pd catalysts originates from the smaller barrier for hydrogenation of ethylene compared with that for its desorption, as reported by Teschner et al.7 and Studt et al.8 Besides, palladium hydride can be readily formed during acetylene hydrogenation,9-10 and because of the hydridic hydrogen, surface ethylene can be readily further hydrogenated.11 In principle, if the adsorption of ethylene is weakened and/or the formation of hydride is inhibited, a higher selectivity toward ethylene could be obtained in acetylene hydrogenation. To improve the selectivity of supported Pd catalysts in acetylene hydrogenation, carbon monoxide and some other molecules have been used as modifiers to compete with ethylene for adsorption sites and favor desorption of ethylene.12 However, the presence of CO reduces the surface concentration of hydrogen and facilitates the formation of green oil and the deactivation of catalysts.13-14 Alternatively, a second metal has been introduced to modify the electronic and geometric structure of the Pd catalysts.15-18 For example, Ag in the Pd catalyst was found to decrease the amount of absorbed hydrogen and suppress the diffusion of hydrogen from bulk to surface, and as a result increase the selectivity to ethylene.19 Cu in the Pd catalyst was shown to decrease the number of multi-coordination Pd sites which are responsible for the formation of ethane and the low selectivity to ethylene.20 The Pd-based intermetallic catalysts have recently shown superior catalytic properties. This is because the active Pd sites are sufficiently isolated and fewer multi-coordination Pd sites are left.21-22 Recently, Feng et al. reported that the (110) surface of Pm3m PdIn intermetallic with single Pd sites exhibited higher selectivity for acetylene hydrogenation than the (111) surface of P4/mmm Pd3In intermetallic with Pd trimer sites.23 Luo et al


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prepared an unsupported intermetallic compound InPd2 by melting and annealing the two metals at a high temperature, and confirmed that the selectivity toward ethylene is governed mainly by the active-site isolation.24 Both acetylene conversion and selectivity to ethylene increased with temperature when it is below 240 oC. Moreover, the specific activity of Pd in InPd2 is much higher than that of elemental Pd, which is very promising for industrial application. However, the low mass activity (activity based on the mass of active metal) of unsupported intermetallic compounds limits the industrial application owing to the low dispersion of palladium. The common method to improve the dispersion and hence the mass activity of the noble metal is to employ a support to disperse the noble metal.25 To date, very little has been explored the catalytic performance of supported intermetallic Pd-In catalysts. In addition, the role of indium in the supported bimetallic Pd-In catalyst may be different from that in the unsupported one due to the particle size effect and the presence of support. Underlying nature of the effect of intermetallic structure and properties on selective hydrogenation needs to be explored to gain a better understanding of the structure, property and performance relationship and thus design better industrial catalysts. Moreover, no investigation has yet been carried out into the formation of green oil over supported bimetallic Pd-In catalyst or into the stability of catalyst, although this understanding is of importance to the industrial application. To this end, we employed the co-impregnation method, which is commonly used to prepare supported noble metal catalyst, to prepare supported Pd-In nanoparticles on Al2O3 (Pd-In/Al2O3). This catalyst was then evaluated at temperatures from 30-70 oC, which is the temperature window for industrial operation, together with Pd/Al2O3 as a reference. The formation of green oil over catalysts was also analyzed with TG-DTA and pyrolysis GC-MS. In this work, we show for the first time that, compared with Pd/Al2O3, Pd-In/Al2O3 exhibits not only higher activity but also higher selectivity. Moreover, the stability is greatly improved by retarding the formation of green oil. Combined catalyst characterization, kinetic study and DFT investigation reveal the underlying nature of the structure-property-performance relationship. In was found to promote the Pd active sites mainly by electronic modification, and this promotion effect is dependent on the amount of In in the bimetallic Pd-In catalyst.


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2. Experimental and Computational methods

2.1 Materials Pseudo-boehmite (Pural SB, Sasol Germany), nitric acid (65%, Shanghai Lingfeng Chemicals), PdCl2 (Sinopharm Chemical Reagent Co. Ltd), hydrochloric acid (37%, Shanghai Lingfeng Chemicals) and indium chloride tetrahydrate (Sinopharm Chemical Reagent Co. Ltd) were used as received without further purification. Deionized water with an electrical conductivity < 10-6 S/cm was used in all experiments.

2.2 Catalysts preparation Pseudo-boehmite was dissolved in deionized water followed by addition of an appropriate amount nitric acid under vigorously stirring at room temperature. The mixture was further stirred vigorously for several hours to obtain aluminum sol. After drying at 80 °C overnight and calcining at 1200 °C for 4 h, Al2O3 support was obtained. The Pd-In/Al2O3 catalyst and monometallic Pd/Al2O3 catalyst were prepared with the incipientwetness co-impregnation method. The Al2O3 support was dried at 120 °C for 2 h prior to use. For the monometallic Pd/Al2O3 catalyst, 1.00 g Al2O3 support was impregnated with a certain amount of aqueous solution of chloropalladic acid to ensure a nominal Pd loading of 0.5 wt.% at room temperature. After aging for 12 h, the precursor was dried at 120 °C for 12 h and then calcined at 300 °C for 2 h, followed by calcining at 500 °C for 2 h. The solid was ground and sieved before use. For the Pd-In/Al2O3 catalyst, the chloropalladic acid solution was replaced with a mixture of chloropalladic acid and indium chloride solution according to the loadings of Pd and In (Pd: 0.5 wt.%, In: 0.4 wt.%).

2.3 Catalysts characterization X-ray diffraction (XRD) characterization of support and catalysts samples were carried out on Rigaku 2550 VB/PC diffractometer with Cu-Kα radiation at 40 kv and 100 mA. The data were collected in the 2θ range of 10°-80° with a scan speed of 12°/min. The Pd and In contents of the samples were determined by inductively


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coupled plasma atomic emission spectrometer (ICP-AES) on Varian 710-ES (Agilent Technologies). TG-DTA were performed on Perkin Elmer Pyris 1 TGA from room temperature to 700 °C at a heating rate of 10 °C/min. Elemental analysis was carried out on a Elementar Vario ELIII elemental analyzer. The transmission electron microscopy (TEM) images were collected with JEOL JEM-2100 transmission electron microscope with an acceleration voltage of 200 kV. The high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) images were performed on a FEI Tecnai G2 F20 S-Twin microscopy operated at 200 kV. The X-ray Photoelectron Spectrum (XPS) measurements of catalysts were carried out on a Kratos XSAM-800 spectrometer with an Al Kα anode (pass energy: 40 eV). The binding energies were calibrated based on C 1s peak at 284.6 eV for all samples. Analysis of green oil composition was performed on pyrolysis GC-MS (Agilent 7890A GC/5975C MSD) equipped with an HP-5MS column as reported in our previous work.26 Hydrogen temperature-programmed reduction (H2-TPR), hydrogen chemisorption, temperature-programmed hydride decomposition (TPHD) and C2H4-TPD were performed on Micrometrics Autochem 2920 chemisorption instrument equipped with a thermal conductivity detector (TCD). For the H2-TPR measurements, about 200 mg catalyst was loaded in a quartz U-tube reactor and reduced under 5% v/v H2/Ar with 30 ml/min from 45 oC to 800 oC with a heating rate of 10 oC/min. Prior to the pulse hydrogen chemisorption measurements, about 100 mg catalyst was reduced in 30 ml/min 5% v/v H2/Ar at 150 oC for 1 h and then hydrogen was desorbed in UHP argon at 180 oC prior to cooling to 40 oC in UHP argon. The average dispersion of Pd crystallites was calculated as described elsewhere.27 The temperature-programmed hydride decomposition was performed according to the reference.6 About 100 mg catalyst was reduced under 30 ml/min 5% v/v H2/Ar at 150 oC for 1 h prior to the TPHD test. For C2H4-TPD measurements, about 100 mg of catalyst was reduced as same as TPHD test and then the reduced sample was purged with He at 200 oC. The catalysts were kept in a flow of C2H4 for 1 h to ensure a saturated adsorption. Afterwards, a flow of He was used to remove the weakly adsorbed C2H4 on catalysts and then the TPD process was carried out from 45 oC to 600 oC at a rate of 10 oC/min. Diffusion reflectance infrared Fourier transform spectroscopy Fourier transform infrared spectra of CO (CODRIFTS) and C2H4 (C2H4-DRIFTS) adsorbed on catalysts were collected on Perkin Elmer Spectrum 100 FTIR spectrometer equipped with a liquid nitrogen cooled Mercury-Cadmium-Telluride (MCT) detector and an in


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situ diffuse reflection cell (Harrick Praying Mantis). All the CO-DRIFTS spectra were recorded at 25 °C with a spectra resolution of 4 cm-1 and accumulation of 32 scans. The powder catalyst samples (about 50 mg) were reduced in pure H2 at 20 ml/min for 1.5 h at 150 °C and then cooled to 25 °C in pure argon at 20 ml/min prior to recording a background spectrum. Thereafter, the reduced samples were treated with 2% v/v CO/Ar at 20 ml/min for 30 min to ensure the steady-state condition and then purged with argon at 20 ml/min until no more gas-phase CO detected in the FTIR spectra before collecting spectrum of CO adsorption on samples. For C2H4-DRIFTS spectra, the sample was also reduced as that in CO-DRIFTS. Thereafter, the sample was exposed under ethylene (20 ml/min) for 60 min followed by evacuated with Ar (20 ml/min) for 60 min. The spectra were collected continuously during the process.

2.4 Catalyst evaluation

Selective hydrogenation of acetylene were carried out on a µBenchCAT reactor (Altamira Instruments, USA) equipped with a stainless steel reactor. Typically, approximate 50 mg catalyst precursor and 500 mg quartz sand were mixed and loaded in the center of stainless steel tube. The mixture was reduced in 50% v/v H2/N2 with a flow rate of 40 ml/min at 150 °C for 2 h and then cooled down to 30 °C in UHP nitrogen. Thereafter, the pressure in reactor was increased to 2.1 MPa under UHP nitrogen prior to feeding the reactor with a reactant stream: 0.6 vol.% acetylene, 1.8 vol.% hydrogen and balance nitrogen. The flow rate of the reactant mixture was 120 ml/min, and the reactor temperature was varied from 30 °C to 70 °C in order to obtain different acetylene conversion. Prior to analysis of gas component, the sample was maintained at each temperature for 1 h to ensure steady-state condition. In order to obtain turnover frequency (TOF) values, the 20 mg catalysts were tested for acetylene hydrogenation at room temperature to under a low acetylene conversion ( L-Pd-In/Al2O3> Pd-In/Al2O3. The more positive H2 dependency of Pd/Al2O3 also suggests the H2-starved Pd surfaces, which is in good


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accordance with the competitive adsorption of both H2 and C2H2 on the active sites in the LangmuirHinshelwood mechanism. The TOF for acetylene hydrogenation based on metal surface area measured by hydrogen chemisorption for bimetallic Pd-In catalysts was plotted as a function of the atomic ratio of In to Pd. As seen in Figure 13A, the value of TOF shows a strong dependence on the In/Pd atomic ratio, i.e., the composition of the catalysts, and the optimum appears at In/Pd atomic ratio of 0.8. The activation energy for Pd/Al2O3 catalyst is ca. 28 kJ/mol, close to the experimental value as previously reported.43 The dependence of activation energies on the In content of the bimetallic Pd-In catalysts is opposite to that of TOFs; the lowest activation energy was found on catalysts with an In/Pd atomic ratio of 0.8. Ethylene selectivity increases concurrently with the In/Pd atomic ratio. To further reveal the origins of composition-dependent performance, CO-DRIFTS, TPHD and XPS characterizations were carried out for H-Pd-In/Al2O3 and L-Pd-In/Al2O3. The peak of hydride decomposition is only observed on L-Pd-In/Al2O3 (Figure 13B), and the H/Pd was calculated to be 0.043 which is smaller than 0.149 of Pd/Al2O3. The hydride could promote the hydrogenation of acetylene to ethane, thus the selectivity of L-Pd-In/Al2O3 is lower than those of Pd-In/Al2O3 and H-Pd-In/Al2O3 but still higher than that of Pd/Al2O3 (Figure 13A and Figure S12). In addition, the Pd0 3d5/2 peak of L-Pd-In/Al2O3 locates at 335.2 eV which is higher than that of Pd-In/Al2O3 (Figure 13C), indicating an insufficient electron density of Pd sites. As discussed above, the electron transfer from In to Pd could weaken the adsorption strength of acetylene and ethylene. Thus, the adsorption of acetylene on L-Pd-In/Al2O3 is stronger than that on Pd-In/Al2O3, which results in more crowded surface sites. The activation of hydrogen on the crowded surface would be more difficult, thus leading to decreased activity, which is in coincident with the kinetics results. Besides, the stronger adsorption of ethylene on L-Pd-In/Al2O3 could easily form ethane via the full hydrogenation.


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Figure 13. (A) Turnover frequency of acetylene conversion (black), ethylene selectivity at 30 oC pressures of C2H2 and H2 (orange) and activation energy (blue) as a function of the In/Pd atomic ratio. (B) TPHD profiles of L-Pd-In/Al2O3 (a), Pd-In/Al2O3 (b) and H-Pd-In/Al2O3 (c). (C) Pd 3d XPS spectra of L-Pd-In/Al2O3 (a), PdIn/Al2O3 (b) and H-Pd-In/Al2O3 (c). As seen in Figure 13C, the Pd0 3d5/2 peak of H-Pd-In/Al2O3 shifts to 334.7 eV, which is 0.1 eV lower than that of Pd-In/Al2O3, suggesting a slightly richer electron density of Pd sites and thus weaker adsorption strength. Moreover, the high In/Pd atomic ratio in H-Pd-In/Al2O3 leads to an obvious geometric isolation as shown in Figure S13, which further weakens the adsorption strength of the surface so that acetylene and hydrogen cannot be effectively activate,64 thus resulting in the decreased activity. It is also confirmed by the aforementioned kinetics investigation. On the other hand, the isolation of contiguous Pd active sites and


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electron-rich active sites in H-Pd-In/Al2O3 promote the adsorption of ethylene and enhance ethylene selectivity. Thus, the composition-dependent performance mainly originates from the different extent of electronic and/or geometric modification for Pd active sites.

4. Conclusion Intermetallic Pd-In nanoparticles were successfully prepared on Al2O3 by the impregnation method. The mass activity of Pd-In/Al2O3 was several magnitudes higher than that of unsupported intermetallic compounds. Also, Pd-In/Al2O3 exhibited higher activity for selective hydrogenation of acetylene and higher selectivity to ethylene than Pd/Al2O3. Adding In into the Pd forms Pd-In (110) intermetallic structure, leading to isolation of Pd sites and electron transfer from In to Pd to form negatively charged Pd surfaces. It resulted in weaker adsorption of acetylene and ethylene as well as suppression of hydride formation. The promoted activation of hydrogen, owing to the weak adsorption of acetylene on Pd-In/Al2O3 together with the decreased particle size contributed to the enhanced activity of Pd-In/Al2O3. The weakened adsorption of ethylene together with absence of hydride leads to the higher selectivity of the Pd-In/Al2O3 catalyst. Moreover, the formation of green oil was retarded by the presence of In, which contributes to the improved stability of the catalyst against green oil formation. The performance of the bimetallic Pd-In catalysts strongly depended on the In/Pd atomic ratio, i.e., the composition of the catalyst, and the optimum appeared at 0.8 of In/Pd ratio. The structural characterization and kinetics investigation indicated that composition-dependent performance originated from the different extent of electronic and/or geometric modification of Pd active sites in bimetallic catalysts. This improved understanding creates more potential for the industrial application of In-promoted palladium catalysts.

ASSOCIATED CONTENT

Supporting Information

The following files are available free of charge. HAADF-STEM images for Pd-In/Al2O3; reproducibility of


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acetylene conversion and ethylene selectivity at different reaction temperature; Arrhenius plots for catalyst; details of H2-Chemisorption and model of Pd and PdIn surfaces; further structural characterizations and catalytic performance of L-Pd-In/Al2O3 and H-Pd-In/Al2O3; details of catalytic performance of different catalysts reported in references; mass transfer calculations for acetylene hydrogenation on Pd/Al2O3 and PdIn/Al2O3 (PDF).

AUTHOR INFORMATION *Corresponding Author Xinggui Zhou Tel: +86-21-64253509; Fax: +86-21-64253528; Email: [email protected]; De Chen Tel: +47-735-93149; Fax: +47-735-95047; Email: [email protected]

Notes The authors declare no competing financial interest.

ACKNOWLEDGMENT This work was financially supported by the National Basic Research Program of China (973 Project, 2012CB720500) and National Natural Science Foundation of China (NSFC, 21376076, 91645122).

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