Uniform NiPx nanospheres loaded onto defective HxWO3-y with three-dimensionally ordered macroporous structure for photocatalytic nitrogen reduction

Uniform NiPx nanospheres loaded onto defective HxWO3-y with three-dimensionally ordered macroporous structure for photocatalytic nitrogen reduction
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均匀的 NiPx 纳米球负载到具有三维有序大孔结构的缺陷 HxWO3-y 上用于光催化氮还原

DOI:
10.1016/j.apcatb.2021.120468
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发表时间:
2021-11
影响因子:
22.1
通讯作者:
Xiaoqing Yan
Xiaoqing Yan
中科院分区:
化学1区
文献类型:
--
作者:
Xiaoling Ren;Ben Chong;Nathan Wells;Guidong Yang;Mengyang Xia;Xiaoqing Yan

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氨合成从N2和水可以实现在温和的条件下利用N2,然而,高活化能的氮加上低的电子-空穴分离效率的光催化剂导致在一个低的氨生成速率。本工作构建了具有氧空位的三维有序大孔结构(3DOM)HxWO 3-y,促进了氮的活化,增加了载流子的分离,从而提高了光催化还原氮的能力,其值为7.4 μmol g−1h−1。通过将NiPx纳米球负载到3DOM结构上,3DOM HxWO 3-y的氮还原能力进一步提高到34 μmol g−1h− 1,是3DOM HxWO 3-y的2.5倍。密度泛函分析表明,HxWO 3-y中的氧空位对N2具有较高的吸附活化能力,氮还原反应(NRR)以对称交替的方式进行.该研究为利用太阳能固氮提供了一条有前途的途径。
Ammonia synthesis from N2and water can be achieved at mild conditions utilizing photocatalysis, however the high activation energy for nitrogen coupled with low electron-hole separation efficiency in the photocatalyst results in a low rate of ammonia generation. In this work, a three-dimensional ordered macroporous structure (3DOM) HxWO3-ywith oxygen vacancies was constructed, which promoted the activation of nitrogen and increased charge carrier separation, thus improving the photocatalytic nitrogen reduction ability with a value of 7.4 μmol g−1h−1. The nitrogen reduction ability of 3DOM HxWO3-ywas further improved to 34 μmol g−1h−1by loading NiPxnanospheres onto the 3DOM structure, which is ∼5 times than 3DOM HxWO3-y. DFT analysis revealed that the oxygen vacancies in HxWO3-yshowed higher adsorption activation ability of N2with the nitrogen reduction reaction (NRR) proceeding in a symmetrical alternating pathway. This study offers a promising route for the N2fixation using solar energy.
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