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Phosphorus-Containing Mesoporous Carbon Acid Catalyst for Methanol Dehydration to Dimethyl Ether
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2019-03-04 , DOI: 10.1021/acs.iecr.8b05897
María José Valero-Romero 1 , Elisa María Calvo-Muñoz 1 , Ramiro Ruiz-Rosas 1 , José Rodríguez-Mirasol 1 , Tomás Cordero 1
Affiliation  

Catalytic dehydration of methanol on an acid carbon catalyst prepared by chemical activation of olive stone with H3PO4 is reported. This preparation methodology produces carbons with a well-developed porous texture and highly thermally stable phosphorus surface complexes in the forms of C–O–PO3 and C–PO3. These P groups confer the carbon with a high oxidation resistance, surface acid, and redox sites. In the absence of oxygen, the catalyst experiment demonstrated a gradual deactivation due to coke deposition on the strong acid sites (P–OH) and reduction of the moderate-strength acid P-surface groups (from C–O–P to C–P type ones). The novelty of this research concerns the high catalytic stability in air atmosphere of this type of carbon with a steady-state methanol conversion of 20% at 300 °C and selectivity towards dimethyl ether of 95%. The presence of oxygen in the reaction gas avoids coke deposition by continuous (re)oxidation of reduced P-surface groups, without gasification of the carbon catalyst.

中文翻译:

含磷介孔碳酸催化剂用于甲醇脱水制二甲醚

报道了在通过用H 3 PO 4对橄榄石进行化学活化而制备的酸性碳催化剂上甲醇的催化脱水。这种制备方法产生的碳具有发达的多孔质地和高度热稳定的磷表面配合物,形式为C–O–PO 3和C–PO 3。这些P基团使碳具有高的抗氧化性,表面酸和氧化还原位点。在没有氧气的情况下,催化剂实验表明,由于焦炭沉积在强酸位点(P–OH)上,并且中等强度的酸性P表面基团(从C–O–P到C–P)的还原,其逐渐失活键入一个)。这项研究的新颖性涉及这种类型的碳在空气中的高催化稳定性,其在300°C下的稳态甲醇转化率为20%,对二甲醚的选择性为95%。反应气体中氧气的存在避免了还原的P-表面基团的连续(再)氧化,而不会使碳催化剂气化,从而避免了焦炭沉积。
更新日期:2019-03-04
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