Superior FeNi3-FeOx/Ni-foam catalyst for gas-phase hydrogenation of dimethyl oxalate to ethanol
Superior FeNi3-FeOx/Ni-foam catalyst for gas-phase hydrogenation of dimethyl oxalate to ethanol
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用于草酸二甲酯气相加氢制乙醇的优质 FeNi3-FeOx/Ni-foam 催化剂
DOI：
10.1016/j.apcatb.2020.118873
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发表时间：
2020
期刊：
影响因子：
--
通讯作者：
Lu Yong
中科院分区：
文献类型：
--
作者：
Zhu Jian;Zhao Guofeng;Sun Weidong;Nie Qiang;Wang Song;Xue Qingsong;Liu Ye;Lu Yong
研制了一种高性能泡沫镍结构fei3 - feox纳米复合催化剂，用于合成气气相草酸二甲酯（DMO）加氢合成乙醇（EtOH）。将水热合成的Ni(OH)2/Ni-foam用硝酸铁（III）水溶液浸渍，在550℃下焙烧（以充分形成NiFe2O4-NiO复合材料），然后在H2中还原，得到优选的FeNi3-FeOx/Ni-foam-(550/350)催化剂。该催化剂在230°C和2.5 MPa条件下，以0.44 h - 1的whsvdmoh和90的H2/DMO摩尔比，以98%的乙醇选择性完全转化DMO，特别是在至少700小时内保持稳定。在180°C条件下，转化率达到88.8 h - 1的高频率。实际上，我们的NiFe2O4-NiO衍生策略使催化剂在feni3纳米合金（~ 16 nm）和FeOxfragments（作为酸位）之间具有丰富的界面，实现了对DMO中的酯基和形成的羟基的协同催化，从而显著提高了其加氢到EtOH的速度。
A high-performance Ni-foam-structured FeNi3-FeOxnanocomposite catalyst is developed for the ethanol (EtOH) synthesis from syngas via gas-phase dimethyl oxalate (DMO) hydrogenation. The hydrothermally-synthesized Ni(OH)2/Ni-foam was impregnated with aqueous solution of iron(III) nitrate, from which the preferred FeNi3-FeOx/Ni-foam-(550/350) catalyst was obtainable by calcining preferably at 550 °C (to adequately form NiFe2O4-NiO composites) and subsequently reducing in H2. Such catalyst is capable of fully converting DMO with 98 % ethanol selectivity at 230 °C and 2.5 MPa using a WHSVDMOof 0.44 h−1and a H2/DMO molar ratio of 90, and particularly, being stable for at least 700 h. A high turnover frequency of 88.8 h−1is achieved at 180 °C. Exactly, our NiFe2O4-NiO derivation strategy endows the catalyst with plentiful interface between FeNi3nanoalloy (∼16 nm) and FeOxfragments (acting as acid sites), achieving synergistic catalysis to ester groups in DMO and as-formed hydroxyl groups, thereby markedly improving its hydrogenation to EtOH.