Selective hydrogenation of CO2 to methanol catalyzed by Cu supported on rod-like La2O2CO3†,Catalysis Science & Technology

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Selective hydrogenation of CO2 to methanol catalyzed by Cu supported on rod-like La2O2CO3†
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2018-01-04 00:00:00 , DOI: 10.1039/c7cy01998j
Kun Chen _{1,

2,

3,

4,

5} , Xinping Duan _{1,

2,

3,

4,

5} , Huihuang Fang _{1,

2,

3,

4,

5} , Xuelian Liang _{1,

2,

3,

4,

5} , Youzhu Yuan _{1,

2,

3,

4,

5}

Affiliation

Cu-based catalysts have long been applied to convert CO₂ and H₂ into methanol, and their performances are well known to be markedly influenced by the support and promoter. Herein, several Cu-based catalysts supported on lanthanum oxides were fabricated by varying the preparation methods and characterized by XRD, TEM, ICP-AES, N₂ physisorption, N₂O chemisorption, CO₂ chemisorption, XPS, and CO₂-TPD. The results showed that the as-prepared Cu supported on rod-like La₂O₂CO₃ (La₂O₂CO₃-R) exhibited the highest TOF_Cu, methanol selectivity and yields of methanol for the hydrogenation of CO₂ to methanol. Distinct from conventional promoter addition, the local formation of a new type of Cu^δ+ species at Cu/La₂O₂CO₃-R interfaces and the original adsorption performance of basic oxides are the two key factors relating to the catalytic performance. Cu supported on La₂O₂CO₃-R with a higher content of Cu^δ+ species and a stronger adsorption for CO₂ leads to superior catalytic activities. DRIFTS studies revealed that the generation of synergetic basic sites at the interfacial areas can increase the intrinsic activity of Cu-based methanol catalysts by moderately and selectively stabilizing methanol synthesis intermediates. This work provides new insights into CO₂ activation over basic oxide-supported Cu catalysts, and the identification of metal–support interactions between Cu and lanthanum oxides is beneficial for the rational design of stable Cu-based catalysts.

中文翻译：

棒状La ₂ O ₂ CO ₃†上负载的Cu催化 CO ₂选择性加氢成甲醇。

铜基催化剂长期以来一直用于将CO ₂和H ₂转化为甲醇，众所周知，其性能会受到载体和助催化剂的显着影响。本文中，通过改变制备方法来制备负载在氧化镧上的几种Cu基催化剂，并通过XRD，TEM，ICP-AES，N ₂物理吸附，N ₂ O化学吸附，CO ₂化学吸附，XPS和CO ₂ -TPD进行表征。结果表明，负载在棒状La ₂ O ₂ CO ₃（La ₂ O ₂ CO ₃ -R）上的_Cu的TOF _Cu最高。，甲醇选择性和将CO ₂加氢成甲醇的甲醇收率。与常规助催化剂的添加不同，在Cu / La ₂ O ₂ CO ₃ -R界面上局部形成新型^{Cuδ +}物种和碱性氧化物的原始吸附性能是与催化性能有关的两个关键因素。负载在La ₂ O ₂ CO ₃ -R上的Cu具有较高的^Cuδ⁺种类含量和对CO ₂的强吸附性导致优异的催化活性。DRIFTS研究表明，在界面区域产生协同碱性位点可以通过适度和选择性地稳定甲醇合成中间体来提高Cu基甲醇催化剂的内在活性。这项工作为碱性氧化物负载的铜催化剂上的CO ₂活化提供了新的见解，而铜与镧氧化物之间金属-载体相互作用的鉴定对于稳定铜基催化剂的合理设计是有益的。

更新日期：2018-01-04

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