Applied Catalysis B: Environment and Energy ( IF 20.2 ) Pub Date : 2022-07-20 , DOI: 10.1016/j.apcatb.2022.121752
Guimei Liu , Ziqian Tang , Xiangkui Gu , Nan Li , Haiqin Lv , Ying Huang , Yubin Zeng , Mingzhe Yuan , Qingguo Meng , Yingtang Zhou , Chuanyi Wang
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Bi-defective g-C3N4 (K and -CN) nanorod arrays with favorable light absorption through multiple light scattering/reflections were designed for photocatalytic N2 reduction. The highest record of NH3 production, 23.5 mmol/(h·gcat), was achieved when dual defects are present at the nanoarrays without any cocatalysts, which is about two orders higher than its counterpart. The N2 reduction rate is proportional to -C
N, unveiling its role as active sites. Its synergistic effect with K was observed. Theoretical calculations support that -C
N site is crucial to N2 activation by donating electrons, while cation like K center traps electrons. Consequently, modification with such dual defects in conjunction with nanoarray configuration creates a favorable electron-dominated structure to overcome the energy barrier for activating inert nitrogen, enhancing charge separation and light absorption effectively. The present work underlines the impetus of defects engineering and nanoarray configuration for the rational design of active photocatalysts for efficient N2 fixation.
中文翻译:
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通过石墨氮化碳纳米棒阵列上的双缺陷-CN 和 K 掺杂位点促进光催化氮还原为氨
双缺陷gC 3 N 4 (K 和-C N) 纳米棒阵列通过多次光散射/反射具有良好的光吸收,被设计用于光催化N 2还原。NH 3产量的最高记录为23.5 mmol/(h·g cat ),这是在没有任何助催化剂的情况下在纳米阵列上存在双重缺陷时实现的,这比其对应物高约两个数量级。N 2还原率与-C N 成正比
,揭示了其作为活性位点的作用。观察到其与 K 的协同作用。理论计算支持-C
N 位点对N 2至关重要通过捐赠电子激活,而像 K 中心这样的阳离子捕获电子。因此,用这种双重缺陷与纳米阵列配置相结合的修饰创造了一种有利的电子主导结构,以克服激活惰性氮的能垒,有效地增强电荷分离和光吸收。目前的工作强调了缺陷工程和纳米阵列配置对合理设计用于高效 N 2固定的活性光催化剂的推动作用。