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碳-钨酸杂化物上高效的太阳能驱动固氮

Efficient Solar-Driven Nitrogen Fixation over Carbon-Tungstic-Acid Hybrids.

作者信息

Li Xiaoman, Wang Wenzhong, Jiang Dong, Sun Songmei, Zhang Ling, Sun Xiang

机构信息

Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.

出版信息

Chemistry. 2016 Sep 19;22(39):13819-13822. doi: 10.1002/chem.201603277. Epub 2016 Aug 18.

Abstract

Ammonia synthesis under mild conditions is of supreme interest. Photocatalytic nitrogen fixation with water at room temperature and atmospheric pressure is an intriguing strategy. However, the efficiency of this method has been far from satisfied for industrialization, mainly due to the sluggish cleavage of the N≡N bond. Herein, we report a carbon-tungstic-acid (WO ⋅H O) hybrid for the co-optimization of N activation as well as subsequent photoinduced protonation. Efficient ammonia evolution reached 205 μmol g  h over this hybrid under simulated sunlight. Nitrogen temperature-programmed desorption revealed the decisive role of carbon in N adsorption. Photoactive WO ⋅H O guaranteed the supply of electrons and protons for subsequent protonation. The universality of carbon modification for enhancing the N reduction was further verified over various photocatalysts, shedding light on future materials design for ideal solar energy utilization.

摘要

在温和条件下合成氨极具吸引力。在室温及大气压下利用水进行光催化固氮是一种引人关注的策略。然而,该方法的效率远不能满足工业化需求,主要原因是N≡N键的裂解缓慢。在此,我们报道了一种用于协同优化氮活化及后续光致质子化的碳 - 钨酸(WO₃·H₂O)杂化物。在模拟太阳光下,该杂化物的氨析出效率达到205 μmol g⁻¹ h⁻¹。程序升温脱附表明碳在氮吸附中起决定性作用。光活性的WO₃·H₂O为后续质子化保证了电子和质子的供应。通过各种光催化剂进一步验证了碳修饰对增强氮还原的通用性,为未来理想太阳能利用的材料设计提供了思路。

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