Propane dehydrogenation(PDH)is one of the most effective technologies to produce propene.Non-noble zinc-based catalysts have paid increasing attention because of low cost and nontoxic,compared with industrial Pt and C...Propane dehydrogenation(PDH)is one of the most effective technologies to produce propene.Non-noble zinc-based catalysts have paid increasing attention because of low cost and nontoxic,compared with industrial Pt and Cr-based catalysts.However,they often suffer from limited catalytic activity and poor stability.Here,we introduced moderate Ni into ZnO supported Silicalite-1 zeolite to increase catalytic activity and stability simultaneously.Zn^(2+) was the definite active site and NiZn alloy facilitated the sluggish H recombination into H_(2)via reverse spillover.Furthermore,the introduction of Ni increased Lewis acid strength caused by electron transfer from ZnO to NiZn alloy,contributing to improved stability.For resulted 0.5 NiZn/S-1,propene formation rate was 0.18 mol C_(3)H_(6)·(g Zn)^(-1)·h^(-1) at 550℃,which was above 1.5 times higher than that over Zn/S-1 without Ni.Under stability test,the deactivation of0.5 NiZn/S-1 was 0.019 h^(-1),which was only 1/10 of that over Zn/S-1.展开更多
基金Financial supports by the National Natural Science Foundation of China(22025802)the Haihe Laboratory of Sustainable Chemical Transformations(CYZC202101)。
文摘Propane dehydrogenation(PDH)is one of the most effective technologies to produce propene.Non-noble zinc-based catalysts have paid increasing attention because of low cost and nontoxic,compared with industrial Pt and Cr-based catalysts.However,they often suffer from limited catalytic activity and poor stability.Here,we introduced moderate Ni into ZnO supported Silicalite-1 zeolite to increase catalytic activity and stability simultaneously.Zn^(2+) was the definite active site and NiZn alloy facilitated the sluggish H recombination into H_(2)via reverse spillover.Furthermore,the introduction of Ni increased Lewis acid strength caused by electron transfer from ZnO to NiZn alloy,contributing to improved stability.For resulted 0.5 NiZn/S-1,propene formation rate was 0.18 mol C_(3)H_(6)·(g Zn)^(-1)·h^(-1) at 550℃,which was above 1.5 times higher than that over Zn/S-1 without Ni.Under stability test,the deactivation of0.5 NiZn/S-1 was 0.019 h^(-1),which was only 1/10 of that over Zn/S-1.