Osman Mohamed E, Maximov Vladimir V, Dipheko Tshepo D, Sheshko Tatiana F, Cherednichenko Alexander G, Nikulshin Pavel A, Kogan Victor M
Peoples' Friendship University of Russia, Moscow 117198, Russia.
N.D. Zelinsky Institute of Organic Chemistry RAS, Moscow 119991, Russia.
ACS Omega. 2022 Jun 6;7(24):21346-21356. doi: 10.1021/acsomega.2c03082. eCollection 2022 Jun 21.
In the present study, a series of K-modified CoMoS catalysts with compositions of 10% K, 3.6% Co, and 12 wt % Mo supported over novel commercial activated carbons such as powder materials (DAC and OBC-1) and fiber materials (fabric active sorption (TCA) and nonwoven activated material (AHM)) were prepared and characterized by Brunauer-Emmett-Teller (BET), X-ray fluorescence (XRF), scanning electron microscopy (SEM), SEM-energy dispersive X-ray (EDX), and transmission electron microscopy (TEM). The catalytic activities for higher alcohol synthesis from syngas, conducted at = 300-360 °C, = 5 MPa, GHSV = 760 L h (kg cat), and H/CO = 1.0, were investigated. Cat-TCA and Cat-AHM have shown a filamentous morphology with a strip axial arrangement and that a few longitudinal grooves and many irregular particles are distributed on the fiber surfaces. The degree of entanglement of the strip axial arrangement in AHM was found to be more than that in TCA, thus leading to form tangled MoS slabs on AHM and long linear slabs on TCA with long rim sites. The obtained results revealed that the CO conversion increases in the order Cat-TCA < Cat-OBC-1 < Cat-DAC < Cat-AHM. Ethanol, propanol-1, and methanol are the most predominant alcohol products in the collected liquid products, with the byproducts containing mainly butanol-1, isobutanol, amyl alcohol, and isoamyl alcohol. Cat-DAC and Cat-OBC-1 show higher selectivity toward C, C, propanol-1, butanol-1, isobutanol, and amyl alcohol-1 than Cat-TCA and Cat-AHM. For powdered activated carbons, microporous catalysts inhibited isomerization because the catalyst that contains the highest micropores (Cat-DAC) produced a considerable amount of linear alcohols compared with Cat-OBC-1.
在本研究中，制备了一系列K改性的CoMoS催化剂，其组成为10%K、3.6%Co和12 wt%Mo，负载在新型商业活性炭上，如粉末材料（DAC和OBC-1）和纤维材料（织物活性吸附剂（TCA）和非织造活性材料（AHM）），并通过布鲁诺尔-埃米特-泰勒（BET）法、X射线荧光（XRF）、扫描电子显微镜（SEM）、SEM-能量色散X射线（EDX）和透射电子显微镜（TEM）对其进行了表征。研究了在300 - 360℃、5MPa、气体时空速（GHSV）=760L h⁻¹（kg催化剂）和H₂/CO = 1.0条件下，由合成气合成高级醇的催化活性。Cat-TCA和Cat-AHM呈现出丝状形态，具有条带轴向排列，并且在纤维表面分布有一些纵向凹槽和许多不规则颗粒。发现AHM中条带轴向排列的缠结程度大于TCA中的，从而导致在AHM上形成缠结的MoS板，而在TCA上形成具有长边缘位点的长线性板。所得结果表明，CO转化率按Cat-TCA < Cat-OBC-1 < Cat-DAC < Cat-AHM的顺序增加。乙醇、丙醇-1和甲醇是收集到的液体产物中最主要的醇类产物，副产物主要含有丁醇-1、异丁醇、戊醇和异戊醇。Cat-DAC和Cat-OBC-1对C₂、C₃、丙醇-1、丁醇-1、异丁醇和戊醇-1的选择性高于Cat-TCA和Cat-AHM。对于粉末状活性炭，微孔催化剂抑制了异构化，因为含有最高微孔的催化剂（Cat-DAC）与Cat-OBC-1相比产生了大量的线性醇。
