Affiliation: | 1. Key Lab of Applied Chemistry of Zhejiang Province and Department of Chemistry &, Key Lab of Biomass Chemical Engineering of Ministry of Education and College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China These authors contributed equally to this work.;2. State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, East China University of Science and Technology, Shanghai, 200237 China These authors contributed equally to this work.;3. Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China;4. Key Lab of Applied Chemistry of Zhejiang Province and Department of Chemistry &, Key Lab of Biomass Chemical Engineering of Ministry of Education and College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029 China;5. State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, East China University of Science and Technology, Shanghai, 200237 China;6. Key Lab of Applied Chemistry of Zhejiang Province and Department of Chemistry &, Key Lab of Biomass Chemical Engineering of Ministry of Education and College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310027 China |
Abstract: | The metal surfaces tend to be oxidized in air through dissociation of the O−O bond of oxygen to reduce the performances in various fields. Although several ligand modification routes have alleviated the oxidation of bulky metal surfaces, it is still a challenge for the oxidation resistance of small-size metal nanoparticles. Herein, we fixed the small-size Pd nanoparticles in tin-contained MFI zeolite crystals, where the tin acts as an electron donor to efficiently hinder the oxidation of Pd by weakening the adsorption of molecular oxygen and suppressing the O−O cleavage. This oxidation-resistant Pd catalyst exhibited superior performance in directly synthesizing hydrogen peroxide from hydrogen and oxygen, with the productivity of hydrogen peroxide at ≈10,170 mmol gPd−1 h−1, steadily outperforming the catalysts tested previously. This work leads to the hypothesis that tin is an electron donor to realize oxidation-resistant Pd within zeolite crystals for efficient catalysis to overcome the limitation of generally supported Pd catalysts and further motivates the use of oxidation-resistant metal nanoparticles in various fields. |