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作 者:李娜[1,2] 毛树红 严文君 张静 LI Na;MAO Shuhong;YAN Wenjun;ZHANG Jing(School of Chemical Engineering and Technology,Taiyuan University of Science and Technology,Taiyuan 030024,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China)
机构地区:[1]太原科技大学化学工程与技术学院,山西太原030024 [2]中国科学院山西煤炭化学研究所、煤转化国家重点实验室,山西太原030001
出 处:《燃料化学学报(中英文)》2024年第5期698-706,共9页Journal of Fuel Chemistry and Technology
基 金:太原科技大学博士科研启动基金(20222084);来晋工作优秀博士奖励基金(20232028);国家自然科学基金(22002181);山西省科技合作交流专项基金(202204041101029);山西省基础研究计划(自由探索类)基金(20210302123214)资助。
摘 要:Cu_(2)O具有禁带窄、环境友好和储量丰富等优点,是一种理想的可见光催化剂,然而其光生载流子复合率高和稳定性差等问题限制了Cu_(2)O在光催化领域的实际应用。为此,本文采用光诱导原位技术,以甲醇为碳源、硫酸铜为铜源,一步成功制备了超薄炭壳层包覆的Cu_(2)O复合纳米材料(Cu_(2)O@C)。结果显示,与常规炭包覆方法相比,光诱导原位技术避免了苛刻的反应条件及繁琐的合成步骤对Cu_(2)O半导体结构的破坏,有效保留了Cu_(2)O本征电子结构,使其具有优异的光催化活性及稳定性。同时,Cu_(2)O@C的核壳结构不仅可以钝化半导体表面缺陷和促进光生载流子的分离,而且炭壳层的包覆还可以避免Cu_(2)O纳米颗粒与溶液的直接接触,有效抑制高活性反应中间体对催化剂结构的破坏。与单独的Cu_(2)O纳米颗粒相比,Cu_(2)O@C复合纳米材料在可见光下的光解水产氢活性和稳定性得到显著提高,产氢速率可达1.28 mmol/(g·h),且在连续五次循环稳定性测试中,氢气生成速率无明显变化。Cuprous oxide(Cu_(2)O)is an ideal visible light catalyst owing to its narrow band gap,environmental benignity and abundant storage;however,the fast recombination of photogenerated charge carriers and poor stability of Cu_(2)O has impeded its application in photocatalysis.Herein,we demonstrate that Cu_(2)O@C nanocomposite can spontaneously evolve from a methanol aqueous solution containing cupric ions under the induction of irradiation.Compared with the traditional carbon coating method,the Cu_(2)O@C nanocomposite obtained by the photo-induced in-situ synthesis can reserve superior original characteristics of the semiconductor under mild reaction conditions,promote the charge transfer and enhance the separation efficiency of charge carriers;in addition,the carbon shells can also effectively prevent Cu_(2)O from photo-corrosion.As a result,the Cu_(2)O@C nanocomposite exhibits excellent photocatalytic activity in the hydrogen evolution in comparison with the Cu_(2)O particles;the H2 evolution rate over the Cu_(2)O@C nanocomposite reaches 1.28 mmol/(g·h)under visible light,compared with the value of 0.065 mmol/(g·h)over Cu_(2)O.Moreover,the Cu_(2)O@C nanocomposite displays good cycle stability,viz.,without any deactivation in the catalytic activity after five cycles.
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