CAJ | 학술논문

采用金属有机物化学气相沉积技术(MOCVD)将羰基钌升华至已浸渍 KNO3和 Ba(NO3)2的高比表面石墨(HSAG)上，制备了一系列Ru/HSAG催化剂。采用X射线衍射、透射电镜（TEM）和N2物理吸附等表征手段，考察了催化剂的物相和表面结构性质及氨合成催化活性。结果表明，以化学气相沉积技术制备的催化剂，能使钌均匀地分散于载体中，形成较小的钌粒子，从而得到高活性的氨合成催化剂。羰基钌的加热温度对升华速率有很大影响，但对沉积效果和催化活性没有明显影响，负载的羰基钌含量对催化剂活性有显著影响。羰基钌在130℃开始分解，并在175℃达到最大分解速率，因此合适的升华温度为110~130℃。催化剂的钌负载量（质量分数）从3.2%增至6.0%时，低反应温度（375℃）下，氨合成活性明显提高。在实验负载量范围内，TEM显示钌纳米粒子的粒径变化不大，基本保持在2 nm左右。
채용금속유궤물화학기상침적기술(MOCVD)장탄기조승화지이침지 KNO3화 Ba(NO3)2적고비표면석묵(HSAG)상，제비료일계렬Ru/HSAG최화제。채용X사선연사、투사전경（TEM）화N2물리흡부등표정수단，고찰료최화제적물상화표면결구성질급안합성최화활성。결과표명，이화학기상침적기술제비적최화제，능사조균균지분산우재체중，형성교소적조입자，종이득도고활성적안합성최화제。탄기조적가열온도대승화속솔유흔대영향，단대침적효과화최화활성몰유명현영향，부재적탄기조함량대최화제활성유현저영향。탄기조재130℃개시분해，병재175℃체도최대분해속솔，인차합괄적승화온도위110~130℃。최화제적조부재량（질량분수）종3.2%증지6.0%시，저반응온도（375℃）하，안합성활성명현제고。재실험부재량범위내，TEM현시조납미입자적립경변화불대，기본보지재2 nm좌우。
Ruthenium catalysts supported on high surface area graphite (HSAG), impregnated with KNO3 and Ba(NO3)2,was prepared via metal-organic chemical vapour deposition technology(MOCVD) with tri-ruthenium dodecacarbonyl as the Ru precursor. The catalysts were characterized by X-ray diffraction, N2 physical adsorption and transmission electron microscope. The activity of the Ru catalyst for ammonia synthesis was evaluated. The results showed that the sublimation rate of tri-ruthenium dodecacarbony depends on temperature under vacuum and dark conditions. It is confirmed that uniform dispersion can be achieved via MOCVD route with Ru nanoparticle sizes around 2 nm. As Ru3(CO)12 commences to decompose at 130℃ and reach maximum decomposition rate at 175℃, the sublimation temperature is suggested to be 110-130℃. With the increase in Ru loading from 3.2% to 6.0%, as evidenced by TEM experiments, Ru nanoparticle size keeps unchanged (around 2 nm), while the activity for ammonia synthesis is enhanced dramatically, especially at low temperature (375℃).