Sensors and Actuators B 241 (2017) 895–903
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Hydrogen sensing properties of Pt-Au bimetallic nanoparticles loaded on ZnO nanorods Faying Fan a,b,∗ , Jiajun Zhang c , Jiao Li c , Na Zhang c , RunRun Hong c , Xiaochuan Deng a,b , Pinggui Tang c , Dianqing Li c,∗ a Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, China b Qinghai Engineering and Technology Research Center of Comprehensive Utilization of Salt Lake Resources, Xining 810008, China c State Key Laboratory of Chemical Resource Engineering, Beijing University of Chemical Technology, Beijing 100029, China
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Article history: Received 12 April 2016 Received in revised form 1 November 2016 Accepted 5 November 2016 Available online 6 November 2016 Keywords: PtAu Bimetallic nanoparticles H2 Gas sensing
a b s t r a c t The mono-noble metal nanoparticles are often loaded onto the sensing materials to promote the gas sensing performance of the materils; however, there have been few reports concerning the effect of the multi-metallic nanoparticles on the sensing performance. It is reported that the multi-metallic nanoparticles shows different absorption and catalytic performance from their mono-metal analogues because of the geometric and electronic effect, so it is very necessary to investigate the gas sensing performance of the multi-metallic nanoparticles loaded materials. In this work, the Pt-Au alloying nanoparticles was prepared and supported on the ZnO nanorods, and this hybrid was used as the H2 sensor for the first time. The sensing testing results indicate that the alloying nanoparticles loaded ZnO exhibits higher sensing response than the mono-metallic nanoparticles loaded ZnO. The Pt-Au bimetallic nanoparticles loaded ZnO shows high sensitivity to ppm-level of hydrogen even at room temperature, and the sensing response of (Pt-Au)-loaded ZnO to 250 ppm of H2 is 157, 47, and 9.6 times higher than that of pure ZnO, Pt-loaded ZnO, and Au-loaded ZnO, respectively. This superior performance of the (Pt-Au)-loaded ZnO to H2 is most probably due to the strong adsorption of H2 onto the Pt-Au bimetallic nanoparticles caused by the geometric and electronic effects between the two metals. © 2016 Published by Elsevier B.V.
1. Introduction Hydrogen is an important and promising energy sources because it is renewable, abundant, efficient, and environmentalfriendly, and it is also an important raw material for the industry [1–8]. However, the using of H2 has high risk of explosion if its concentration exceeds 4% in air, and the safety issues will always arise when hydrogen is used or produced [9–12]. Therefore, the development of highly sensitive and fast-detecting hydrogen sensors for the detecting of H2 leakage from storage and transporting equipment is very important and urgent. Semiconductor based gas sensors is one of the most important equipment for the detection of gases, and they have been widely used to detect the H2 S, ethanol, CO, CH4 , NO2 etc. [13–17]; however, the sensitivity to H2 is very low. It is reported that the deposition of noble metal can enhance the H2 sensing performances of sen-
∗ Corresponding authors. E-mail address:
[email protected] (F. Fan). http://dx.doi.org/10.1016/j.snb.2016.11.025 0925-4005/© 2016 Published by Elsevier B.V.
sors due to the strong oxygen dissociation and spillover effect of noble metals with unique electric and catalytic properties and the synergic electronic interaction with the oxide materials [18–22]. Ghim Wei Ho, et al. [23] reported that Pd based sensor has excellent H2 sensing performance. Leu et al. [24] prepared Pd nanoparticles decorated ZnO nanorods with superior sensing properties to the H2 even at room-temperature. Xie et al. [25] also reported that Pt-functionalized NiO nanotubes show superior gas sensing performance. Wang et al. [18] has prepared Au functionalized ZnO nanowires, and the results demonstrated that the sensor with Au functionalized exhibited not only faster response and recovery but also higher sensitivity to benzene and toluene than the pristine ZnO senor. However, the response of those reported sensors to H2 is still low or the operation of these sensors requires high temperature. The bimetallic nanoparticles consisting of two or more components usually exhibit different properties from their mono-metal analogues because of the geometric and electronic effect between the two metals [26–29]. PdAu bimetallic nanoparticles shows excellent stability for the oxygen reduction reaction [30]. Bert D. Chandler et al. reported that incorporating small amounts of Pd into
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supported Au catalysts has been shown to have beneficial effects on selective hydrogenation reactions [31]. In addition, it is reported that the bimetallic materials have showed superior sensing properties to the gases, such as H2 , oxygen, and liquefied petroleum gas [32,33]. Therefore, it is of great interest to investigate the gas sensing properties of the bimetallic nanoparticles modified gas sensing materials. As is well known, the Pt is an excellent hydrogenation and oxygen reduction reaction catalyst [34–37]; while the Au based catalysts have been identified as highly active for many oxidation reactions, such as CO oxidation [38], and the selective oxidation of alcohols [39,40], because of their excellent hydrogen and oxygen adsorption and/or dissociation properties. As the sensing response of the sensor to H2 is defined as the resistance changes of the sensor in air and in H2 , and that depends on the both adsorption of hydrogen and oxygen onto the materials, so it is very necessary to study the effect of the Pt-Au bimetallic nanoparticles on the H2 sensing performance since the coexistence of Pt and Au will promote both the adsorptions of H2 and O2 onto the materials. Herein, we have prepared Pt-Au bimetallic nanoparticles with Pt and Au homogeneously distributed, and then the PtAu nanoparticles were loaded onto the ZnO nanorods. The gas sensing performance of the ZnO-supported Pt-Au nanoparticles (Pt-Au/ZnO) to H2 were tested, and the Pt-Au/ZnO exhibits higher sensing response to H2 than the mono-metal modified ZnO, and the Pt-Au/ZnO also shows high sensing response to H2 even operated at room temperature. 2. Experimental section 2.1. Materials The sodium hydroxide (NaOH), Hexadecyltrimethy Ammonium Bromide (CTAB), zinc nitrate (Zn(NO3 )2 ·6H2 O), H2 PtCl6 &903;6H2 O, HAuCl4 &903;4H2 O, polyvinyl alchol (PVA, MW ≈ 2000), and NaBH4 were analytic grade and used without further purification. The water used in all the experiments was deionized and had an electrical conductivity 7;(Pt + Au)/ZnO > Pt-Au/ZnO > Au/ZnO. This is because the particles size of Pt is smaller than the (Pt + Au), Pt-Au, and Au, and as depicted in XPS results the nanoparticles with smaller size may adsorb more oxygen. Fig. 9(b) presents the real-time change of the resistance for samples in different gas atmospheres. The resistance of the samples maintains in air, but they quickly decrease with the H2 injected into and reached banlance finally. The time taken since the resistance decreases to reaches banlance for Pt-Au/ZnO, (Pt + Au)/ZnO, Pt/ZnO, and Au/ZnO are 115 s, 119 s, 127 s, and 121 s, respectively. The results indicate that the Pt-Au/ZnO spend the shorest time to reach balance, and the samples with shorter response time shows higher sensing response to H2 , this is because of that the response of sensor is strongly correlated to the adsorption properties of the materials, and materials with strong adsorption of H2 shows fast and high sensing response. Thus the high and fast sensing response of Pt-Au/ZnO to H2 is most probably due to the strong adsorption of the H2 by Pt-Au nanoparticles. Literatures reported that the bimetallic nanoparticles show different adsorption and catalytic performances from the monometallic nanoparticles, due to the synergistic and electronic effects of the bimetallic nanoparticles. For the synergistic effect, upon the dilution of Au by Pt, which creates isolated Au and Pt ensumbles on the nanoparticles surface and forms highly active sites, as a
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result, the adsoprtion and catalytic performance of the bimetallic nanoparticles are enhanced [45]. Thus, with the increase of the active sites, the adsorption of H2 may enhance and accelerate. In addition, as we presented in Fig. S2, the bimetallic nanoparticles loaded ZnO shows higher sensing response than the monometallic nanoparticles loaded owing to the synergistic effect of the bimetallic nanoparticles. On the other hand, using ab initio density functional theory, Alberto Striolo et al. investigated that the adsorption of H2 onto the Pt-Au bimetallic nanoparticles can be more favorable than that on monometallic. Because the adsorption of the H2 is dependent on the d-band of the metal, and the Pt 5d band and Au 5d band in the Pt-Au bimetallic becomes narrower and shift closer to the Fermi level compared with the Pt and Au monometallic nanoparticles, which will lead to the strong hydrogen adsorption [53–55]. 4. Conclusions In conclusion, ZnO supported Pt-Au bimetallic nanoparticles has been prepared. The bimetallic nanoparticles with Pt and Au homogeneously distributed are uniformly and stably coated onto the ZnO nanorods, and a gas sensor based on the Pt-Au bimetallic nanoparticles loaded ZnO has been manufactured. The gas sensing testing results indicate that the obtained Pt-Au bimetallic nanoparticles loaded ZnO shows higher sensing response to 250 ppm H2 , which is 9.6 times higher than the ZnO supported Au, 47 times higher than ZnO supported Pt, and 157 times higher than pure ZnO. In addition, the Pt-Au deposited ZnO shows high sensitivity to H2 even at room temperature. What more, the Pt-Au loaded ZnO exhibits higher sensing response to H2 than the Pd-Au loaded ZnO, Pd-Pt loaded ZnO, and Pd-Pt-Au loaded ZnO. This superior performance of the Pt-Au deposited ZnO to H2 is depending on the strong adsorption of H2 onto the Pt-Au bimetallic nanoparticles owing to the synergetic and electronic effects of the two metals. Acknowledgments This work was supported by the National Natural Science Foundations of China, Beijing Engineering Center for Hierarchical Catalysts, the Fundamental Research Funds for the Central Universities (YS1406), Qinghai Science&Technology Projects (2016-ZJ-927Q, 2016-GX-103), and the funds of the Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lake, Chinese Academy of Sciences. References [1] M. Nielsen, E. Alberico, W. Baumann, H.J. Drexler, H. Junge, S. Gladiali, M. Beller, Low-temperature aqueous-phase methanol dehydrogenation to hydrogen and carbon dioxide, Nature 495 (2013) 85–89. [2] J.M. Petersen, F.U. Zielinski, T. Pape, R. Seifert, C. Moraru, R. Amann, S. Hourdez, P.R. Girguis, S.D. Wankel, V. Barbe, E. Pelletier, D. Fink, C. Borowski, W. Bach, N. Dubilier, Hydrogen is an energy source for hydrothermal vent symbioses, Nature 476 (2011) 176–180. [3] L. Schlapbach, A. Zuttel, Hydrogen-storage materials for mobile applications, Nature 414 (2001) 353–358. [4] J.R. Khusnutdinova, J.A. Garg, D. Milstein, Combining low-pressure CO2 capture and hydrogenation to form methanol, ACS Catal. 5 (2015) 2416–2422. [5] Y. Nakagawa, K. Takada, M. Tamura, K. Tomishige, Total hydrogenation of furfural and 5-hydroxymethylfurfural over supported Pd–Ir alloy catalyst, ACS Catal. 4 (2014) 2718–2726. [6] T.P. Lin, J.C. Peters, Boryl-mediated reversible H2 activation at cobalt: catalytic hydrogenation, dehydrogenation, and transfer hydrogenation, J. Am. Chem. Soc. (2013) 15310–15313. [7] Q.A. Chen, M.W. Chen, C.B. Yu, L. Shi, D.S. Wang, Y. Yang, Y.G. Zhou, Biomimetic asymmetric hydrogenation: in situ regenerable hantzsch esters for asymmetric hydrogenation of benzoxazinones, J. Am. Chem. Soc. 133 (2011) 16432–16435. [8] C.M. Zall, J.C. Linehan, A.M. Appel, A molecular copper catalyst for hydrogenation of CO2 to formate, ACS Catal. 5 (2015) 5301–5305.
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Biographies Faying Fan received her PhD degree in 2015 at BUCT. She is a lecturer in the Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lake, Chinese Academy of Sciences. Her research project involves sensing materials and environmentally friendly catalytic materials. Jiajun Zhang is currently pursuing a postgraduate degree at BUCT. His research project involves sensing materials and application. Jiao Li received her postgraduate degree in 2016 at BUCT. Her research project involves sensing materials and application. Na Zhang received her postgraduate degree in 2016 at BUCT. Her research project involves catalytic materials and application. Runrun Hong received her bachelor’s degree from BUCT and is currently pursuing a PhD degree at BUCT. His research project involves environmentally friendly catalytic materials. Xiaochuan Deng is a researcher in the Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lake, Chinese Academy of Sciences. His research interests include the development of new method and technique of salt resource materials application. Pinggui Tang received his PhD degree in 2011 at BUCT. He is a lecturer in the College of Science in BUCT. His research is focused on intercalation chemistry of layered double hydroxides and inorganic functional materials. Dianqing Li received his MS degree in 1989 at Beijing Institute of Chemical Technology and PhD degree in 2001 at Tianjin University. His research interests are the development and application of functional inorganic materials. He is currently a professor in the State Key Laboratory of Chemical Resource Engineering at Beijing University of Chemical Technology (BUCT).
