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具有可调能带结构的超细多孔氮化碳束同时实现太阳能光解水和选择性苯甲醇氧化
作者:小柯机器人 发布时间:2020/11/5 16:26:44

黑龙江大学化学与材料科学学院的付宏刚研究团队经过不懈努力,获得了一种具有可调能带结构的超细多孔氮化碳束,并用其同时实现太阳能光解水和苯甲醇的选择性氧化。 该项研究成果发表在11月3日的《德国应用化学》上。

在这项研究中,课题组通过热解由L-精氨酸和三聚氰胺制备的不对称超分子前体,合成了猕猴桃样氮化碳(ACN)束。ACN束拥有可调带隙(2.25 eV ~ 2.75 eV)和具有超薄孔壁的中空毛细管,这些特点起到了丰富反应位点、提高可见光吸收和电荷分离的作用。在苯甲醇存在的条件下,ACN束展示出优秀的纯水光解能力(95.3 μmol / h),同时在日光照射下,苯甲醇被选择性氧化为苯甲醛(90.9%转化率和99.7%选择性)。

通过2D同位素标记、分离和检测,该反应中释放的氢气中的质子被证实来自于水。在此基础上,研究人员推导出水光解和苯甲醇氧化的机理,有望为在一个系统中同时利用光生电子和空穴提供更多灵感。

据了解,具有多种功能(包括有机合成和水分解)的光催化剂的理性设计充满希望,但也非常具有挑战性。

附:英文原文

Title: Ultrathin Porous Carbon Nitride Bundles with an Adjustable Energy Band Structure toward Simultaneous Solar Photocatalytic Water Splitting and Selective Phenylcarbinol Oxidation

Author: Honggang Fu, Baogang Wu, Liping Zhang, Baojiang Jiang, Qi Li, Chungui Tian, Ying Xie, Weizuo Li

Issue&Volume:03 November 2020

Abstract: Rational design of photocatalysts with multiple functions, including organic synthesis and water‐splitting, is promising and challenging. Herein, we synthesized actiniae‐like carbon nitride (ACN) bundles based on the pyrolysis of an asymmetric supramolecular precursor prepared from L‐arginine (L‐Arg) and melamine. ACN has adjustable band gaps (2.25 eV ~ 2.75 eV) and hollow microtubes with ultrathin pore walls, which enrich reaction sites, improve visible‐light absorption and enhance charge separation. In the presence of phenylcarbinol, ACN exhibited excellent pure water‐splitting ability (95.3 μmol/h) and in the meanwhile phenylcarbinol was selectively oxidized to benzaldehyde (conversion of 90.9%, selectivity of 99.7%) under solar irradiation. For the concurrent reactions,  2D isotope labeling, separation and detection were conducted to confirm that the proton source of released hydrogen is water. Further, we theorized the mechanism of water splitting and phenylcarbinol oxidation and hope that it provides inspiration for simultaneous utilization of photogenerated electrons and holes in one system.

DOI: 10.1002/anie.202013753

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202013753

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:12.959
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx