Promotion of iridium complex catalysts for HCOOH dehydrogenation by trace oxygen
Promotion of iridium complex catalysts for HCOOH dehydrogenation by trace oxygen
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微量氧促进铱络合物催化剂 HCOOH 脱氢
DOI：
10.1134/s002315841705024x
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发表时间：
2017-09
影响因子：
1.1
通讯作者：
Zhou Xiaochun
中科院分区：
文献类型：
--
作者：
Zhan Yulu;Shen Yangbin;Du Ying;Yue Baohua;Zhou Xiaochun
Ir配合物是甲酸脱氢的重要均相催化剂。本文报道了通过微量氧的活化可以大大提高Ir配合物的活性。活化后，异核Ir-Ru催化剂的活性增加了18倍，而单核Ir-Ru催化剂的活性增加了23倍。氧是激活的关键因素。但过高的氧气浓度对活动有负面影响。在HCOOH脱氢过程中，存在Ir络合催化剂活化的最佳H2O2浓度。异核Ir-Ru催化剂的活化需要极低浓度的氧（2.4 × 10-6 M），而单核催化剂则需要更高浓度的氧（290 × 10-6 M）。从研究结果可以推断，复合催化剂的活化是由于化学变化和结构变化的相互作用。这些发现可能有助于提高均相催化剂的催化活性，均相催化剂广泛应用于甲酸脱氢、CO2还原等过程。此外，本文还指出铱配合物是由H2和O2直接合成H2O2的优良催化剂。
Ir complexes are important homogeneous catalysts for formic acid (FA) dehydrogenation. This paper reports that the activity of Ir complexes can be greatly improved through the activation by trace amounts of oxygen. After activation the activity of the heterodinuclear Ir–Ru catalyst increased 18-fold whereas for the mononuclear catalyst a 23-fold increase was observed. Oxygen is the key factor for the activation. But an excessive concentration of oxygen has a negative effect on the activity. There is an optimal concentration of H2O2 for the activation of Ir complex catalysts in HCOOH dehydrogenation. A very low concentration of oxygen (2.4 × 10–6 M) is needed for the activation of the heterodinuclear Ir–Ru catalyst while the mononuclear catalyst requires the presence of oxygen in a much higher concentration (290 × 10–6 M). From the results of the study it can be inferred that the activation of complex catalysts is due to the interplay of chemical and structural changes. These findings may be helpful in the attempts to improve the catalytic activity of homogeneous catalysts, which are widely used in formic acid dehydrogenation, CO2 reduction and in other processes. In addition, this paper indicates that iridium complexes are excellent catalysts for the direct synthesis of H2O2 from the H2 and O2.
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