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High-Yield Production of Deoxygenated Monomers from Kraft Lignin over ZnO-Co/N-CNTs in Water
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2021-02-18 , DOI: 10.1021/acssuschemeng.0c08664
Umair Mushtaq 1 , Jaeyong Park 2 , Asim Riaz 2 , Virendra Ranaware 3 , Muhammad Kashif Khan 2 , Deepak Verma 1, 2, 3 , Jaehoon Kim 1, 2, 3
Affiliation  

Catalytic conversion of technical lignin to value-added chemicals and fuels is important for realizing economically viable lignocellulosic biomass refineries. The choice of catalysts and solvents is critical for the effective conversion of the technical lignin to chemicals and fuels by the cleavage of the C–C bonds. In this study, catalytic depolymerization and hydrodeoxygenation of Kraft lignin (KL) were investigated over bimetallic ZnO and Co deposited on N-doped carbon nanotubes (ZnO-Co/N-CNTs) in an aqueous medium. The catalytic activity of ZnO-Co/N-CNTs was compared with those of various noble and non-noble metal-based catalysts. Almost complete KL conversion with a very low solid residue yield (5 wt %), a high bio-oil yield (52 wt %), a high degree of deoxygenation (DOD, 59.0%), and a high monomeric yield (12.1 wt %) was achieved over ZnO-Co/N-CNTs at 350 °C and 6 h reaction time. The monomers mainly consisted of cyclohexanone and its alkyl-substituted derivatives and alkylated phenols. At 400 °C, the monomeric yield and DOD increased to 24.4 wt %and 61.0%, respectively. In addition, the produced bio-oil exhibited high-calorific values of 34.3–37.0 MJ kg–1 because of the high activity of ZnO-Co/N-CNTs for hydrodeoxygenation. ZnO-Co/N-CNTs outperformed most of the metal-supported catalysts including 5 wt % Pd, 5 wt % Ru, 5 wt % Pt, 66 wt % Ni, and CoMo on various supports of activated carbon and alumina. The use of water as the solvent resulted in much higher bio-oil and monomeric yields than those using methanol, isopropyl alcohol, and n-hexane (12–37 and 3.2–4.1 wt %, respectively). The high bio-oil and monomeric yields with a high DOD in water make ZnO-Co/N-CNTs highly attractive in the development of an environmentally friendly technical lignin conversion process.

中文翻译:

在水中的ZnO-Co / N-CNTs上由牛皮纸木质素高产量生产脱氧单体

工业木质素催化转化为增值化学品和燃料对于实现经济上可行的木质纤维素生物质精炼厂非常重要。催化剂和溶剂的选择对于通过裂解C–C键有效地将工业木质素转化为化学品和燃料至关重要。在这项研究中,研究了牛皮纸木质素(KL)在水介质中沉积在N掺杂碳纳米管(ZnO-Co / N-CNTs)上的双金属ZnO和Co的催化解聚和加氢脱氧。将ZnO-Co / N-CNTs的催化活性与各种贵金属和非贵金属基催化剂的催化活性进行了比较。几乎完全的KL转化,具有非常低的固体残留物收率(5 wt%),高的生物油收率(52 wt%),高的脱氧度(DOD,59.0%)和高的单体收率(12。在350°C和6 h反应时间下,在ZnO-Co / N-CNT上获得了1 wt%的碳。单体主要由环己酮及其烷基取代的衍生物和烷基化的酚组成。在400℃下,单体产率和DOD分别增加至24.4重量%和61.0%。此外,所生产的生物油显示出34.3–37.0 MJ kg的高热值–1是因为ZnO-Co / N-CNT具有加氢脱氧的高活性。在活性炭和氧化铝的各种载体上,ZnO-Co / N-CNT的性能优于大多数金属负载的催化剂,包括5 wt%的Pd,5 wt%的Ru,5 wt%的Pt,66 wt%的Ni和CoMo。作为溶剂使用的水导致高得多的生物油和单体产率比使用甲醇,异丙醇的那些,并且Ñ己烷(12-37和3.2-4.1%(重量),分别地)。水中具有高DOD的高生物油和单体产率使ZnO-Co / N-CNT在开发环保型技术木质素转化工艺中极具吸引力。
更新日期:2021-03-01
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