Hydrogenation of benzoic acid to benzyl alcohol over Pt/SnO2
Hydrogenation of benzoic acid to benzyl alcohol over Pt/SnO2
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DOI：
10.1016/j.apcata.2020.117420
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发表时间：
2020-03-05
影响因子：
5.5
通讯作者：
Hardacre, Christopher
中科院分区：
文献类型：
--
作者：
Chen, Xiaohan;Wang, Ziyun;Hardacre, Christopher
苯甲酸在Pt/SnO2上液相加氢，在温和的反应条件下（苯甲酸转化率为98%时为97%）对苯甲醇有很好的选择性。DFT计算表明，随着SnO2载体的部分还原，苯甲酸的有利吸附模式从芳香环转变为酸性羰基。吸附模式的转换证实了实验观察到的选择性，酸羰基吸附和氢化发生在Pt/SnO2上。通过原位XPS观察到Pt/SnO2的还原形成一定程度的金属锡和Pt的完全还原，这可能导致Pt- sn合金相和/或SnOx迁移到Pt阻塞位点进行环氢化。Pt/SnO2表面未观察到苯的加氢反应或苯甲酸的苯环，而Pt颗粒的界面处存在氧化锡，以激活酸性羰基进行加氢。
Hydrogenation of benzoic acid in the liquid phase over Pt/SnO2 has afforded excellent selectivity to benzyl alcohol under mild reaction conditions (97 % at 98 % conversion of benzoic acid). DFT calculations have shown that the favoured mode of adsorption of benzoic acid switched from the aromatic ring to the acid carbonyl group with partial reduction of the SnO2 support. The switch in adsorption mode corroborates the experimentally observed selectivity with acid carbonyl group adsorption and hydrogenation occurring over Pt/SnO2. Reduction of Pt/SnO2 was observed by in-situ XPS forming a degree of metallic tin and complete reduction of Pt which could lead to Pt-Sn alloy phases and/or migration of SnOx onto Pt blocking sites for ring hydrogenation. No hydrogenation of benzene or the benzene ring of benzoic acid was observed over Pt/SnO2 with oxidic tin species at the interface of Pt particles proposed to activate the acid carbonyl group for hydrogenation.