Promoting the Direct H₂O₂ Generation Catalysis by Using Hollow Pd–Sn Intermetallic Nanoparticles

Abstract

Although direct hydrogen (H ) oxidation to hydrogen peroxide (H O ) is considered as a promising strategy for direct H O synthesis, the desirable conversion efficiency remains formidable challenge. Herein, highly active and selective direct H oxidation to H O is achieved by using hollow Pd-Sn intermetallic nanoparticles (NPs) as the catalysts. By tuning the catalytic solvents and catalyst supports, the efficiency of direct H oxidation to H O can be optimized well with the hollow Pd Sn NPs/P25 exhibiting H O selectivity up to 80.7% and productivity of 60.8 mol kg h . In situ diffuse reflectance infrared Fourier transform spectroscopy of CO adsorption results confirm the different surface atom arrangements between solid and hollow Pd-Sn NPs. X-ray photoelectron spectra results show that the higher efficiency of Pd Sn NPs/P25 is due to its higher content of metallic Pd and higher ratio of Sn , which benefit H O production and selectivity.

Direct Synthesis of Hydrogen Peroxide Using Cs-Containing Heteropolyacid-Supported Palladium–Copper Catalysts

“…We have recently reported that it is possible to significantly enhance the selectivity of Pd-based catalysts towards H2O2 through the encapsulation of small Pd nanoparticles in a suitable secondary metal oxide, removing the requirement of Au incorporation to achieve a highly selective Pd catalyst in the absence of acid or halide stabilizing agents [23]. With subsequent studies further demonstrating the remarkable effects of Pd modification by Sn [24,25]. While others have investigated the beneficial effects of Zn [26], Ni [27], and Te [28] into Pd nanoparticles, with computational studies by Xu et al predicting Pd-Pd and Pd-W as potential candidates for highly active catalysts for the direct synthesis of H2O2 [29].…”

The Selective Oxidation of Cyclohexane via In-situ H2O2 Production Over Supported Pd-based Catalysts

“…In recent years focus has shifted towards alloying Pd with a range of non-precious metals, with numerous studies reporting the enhanced catalytic efficacy achieved through the introduction of Sn [35,36], Ag [37], Zn [38], Ni [39,40], In [41,42], Sb [43], and Te [44] into Pd nanoparticles. Typically, the improved selectivity of the bimetallic catalysts has been attributed to a combination of a reduction of contiguous Pd ensembles and a modification of Pd oxidation state.…”

Advanced Development Strategy of Nano Catalyst and DFT Calculations for Direct Synthesis of Hydrogen Peroxide

“…This idea‐derived new system delivered a significantly high H 2 O 2 selectivity (>90%) as well as a H 2 O 2 productivity of 3660 mol H2O2 kg cat –1 h –1 , which are superior to those provided in a number of previous reports ( Table 4 , Figure 19c,d). [ 12,41,42,76,140,153–161 ] . The completed system also retained nearly 100% of its activity over 100 h of reaction even in high or low concentration of H 2 O 2 (Figures 19e,f).…”