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定制聚合氮化碳的晶界化学以增强太阳能制氢和一氧化碳还原性能。

Tailoring the Grain Boundary Chemistry of Polymeric Carbon Nitride for Enhanced Solar Hydrogen Production and CO Reduction.

作者信息

Zhang Guigang, Li Guosheng, Heil Tobias, Zafeiratos Spiros, Lai Feili, Savateev Aleksandr, Antonietti Markus, Wang Xinchen

机构信息

Max Planck Institute of Colloids and Interfaces, 14476, Potsdam, Germany.

State Key Laboratory of Photocatalysis on Energy and Environment, College of Chemistry, Fuzhou University, Fuzhou, 350116, China.

出版信息

Angew Chem Int Ed Engl. 2019 Mar 11;58(11):3433-3437. doi: 10.1002/anie.201811938. Epub 2019 Feb 12.

Abstract

Photocatalytic water splitting is a promising and clean way to mimic plant photosynthesis in a sustainable manner. Improvements of the quantum efficiency and optical absorption in the relevant range are necessary steps to approach practicality. Herein, we reported that these issues can be readily addressed when 5-aminotetrazole, a monomer with high nitrogen content, is used for the synthesis of carbon nitride. The molten salt mixture NaCl/KCl is used as a high-temperature solvent to tailor the grain boundary structure and chemistry. Visible light quantum efficiency for H production of 0.65 could be obtained in the presence of K HPO as a double layer modifier. This value is very high, considering that this number depends on light to charge couple conversion, charge localization, as well as a successful oxidation and reduction reaction.

摘要

光催化水分解是一种很有前景的、以可持续方式模拟植物光合作用的清洁方法。提高相关范围内的量子效率和光吸收是迈向实用性的必要步骤。在此,我们报道,当使用高氮含量的单体5-氨基四唑用于合成氮化碳时,这些问题可以很容易地得到解决。熔融盐混合物NaCl/KCl用作高温溶剂来调整晶界结构和化学性质。在存在磷酸氢二钾作为双层改性剂的情况下,产氢的可见光量子效率可达0.65。考虑到这个数值取决于光到电荷的耦合转换、电荷定位以及成功的氧化还原反应,这个值是非常高的。

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