CAJ | 학술논문

实验研究了在氢气存在下,一氧化碳与亚硝酸乙酯偶联合成草酸二乙酯反应体系在典型操作条件下的化学反应和反应性能,结果表明氢气只与反应体系中的亚硝酸乙酯反应生成乙醇.由于氢气与一氧化碳在催化剂表面竞争吸附,并且氢的存在打破了生成草酸二乙酯所必需的正常的氧化还原过程:Pd0→Pd2+→Pd0,因此氢的引入使一氧化碳转化率及草酸二乙酯选择性下降.此外,化学吸附测试结果表明氢气和一氧化碳是在催化剂表面同一活性中心上吸附.
실험연구료재경기존재하,일양화탄여아초산을지우연합성초산이을지반응체계재전형조작조건하적화학반응화반응성능,결과표명경기지여반응체계중적아초산을지반응생성을순.유우경기여일양화탄재최화제표면경쟁흡부,병차경적존재타파료생성초산이을지소필수적정상적양화환원과정:Pd0→Pd2+→Pd0,인차경적인입사일양화탄전화솔급초산이을지선택성하강.차외,화학흡부측시결과표명경기화일양화탄시재최화제표면동일활성중심상흡부.
The use of carbon monoxide from coal or natural gas to produce dialkyl oxalate is an important research area in C1 chemical technology. The chemical reactions and performance in the coupling reaction system for synthesis of diethyl oxalate from carbon monoxide and ethyl nitrite were tested in the presence of hydrogen under the typical coupling reaction conditions. The results indicated that hydrogen only reacts with ethyl nitrite to form ethanol. The introduction of hydrogen to the reaction system lowered the conversion of carbon monoxide and the selectivity of diethyl oxalate because hydrogen competed with carbon monoxide to adsorb on the surface of the catalyst and interrupted the normal redox process of Pd0→Pd2+→Pd0 necessary for the formation of diethyl oxalate. Also, the chemisorption measurements revealed that hydrogen and carbon monoxide adsorbed on the same active sites of the catalyst.