<br>氧化铜氢还原的双重机制：表面反应和次表面氧原子转移。,RSC Advances - X-MOL

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氧化铜氢还原的双重机制：表面反应和次表面氧原子转移。
RSC Advances ( IF 3.9 ) Pub Date : 2024-03-26 , DOI: 10.1039/d4ra01240b
Yehan Wu ₁ , Ruixue Fang ₁ , Laihong Shen ₁ , Hongcun Bai ₂

Affiliation

氢气（H2）还原氧化铜（CuO）的研究有助于阐明氧载体的还原机理。本研究通过密度泛函理论（DFT）方法和热力学计算研究了H2还原CuO的机理和氧原子转移过程。 DFT计算结果表明，在H2与CuO表面反应过程中，Cu发生了Cu2+→Cu1+→Cu0转变，Cu2O相的Cu-O键(-IpCOHP=2.41)比(-IpCOHP=2.41)更稳定。 1.94）的CuO相，并且H2还原Cu2O比CuO还原更困难。随着表面氧空位浓度的增加，表面下的O原子更有可能在零H2覆盖率（表面上没有H2分子）转移到表面，从而使表面保持稳定的Cu2O相。然而，当H2覆盖率为0.25单层（ML）（每四个表面Cu原子一个H2分子）时，表面上H原子的存在使得O原子从地下向上转移变得更加困难。还原反应消耗表面O原子的速率大于还原反应引起的次表面O原子转移的速率，表面Cu2O相不能稳定维持。通过热力学分析，在高H2浓度下，H2与CuO反应更容易生成Cu，而在低H2浓度下，更容易生成Cu2O。综上所述，CuO与H2反应过程中Cu的价态取决于H2的浓度。

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Dual mechanisms in hydrogen reduction of copper oxide: surface reaction and subsurface oxygen atom transfer.

The study of the reduction of copper oxide (CuO) by hydrogen (H2) is helpful in elucidating the reduction mechanism of oxygen carriers. In this study, the reduction mechanism of CuO by H2 and the process of oxygen atom transfer were investigated through the density functional theory (DFT) method and thermodynamic calculation. DFT calculation results showed that during the reaction between H2 and the surface of CuO, Cu underwent a Cu2+ → Cu1+ → Cu0 transformation, the Cu-O bond (-IpCOHP = 2.41) of the Cu2O phase was more stable than that (-IpCOHP = 1.94) of the CuO phase, and the reduction of Cu2O by H2 was more difficult than the reduction of CuO. As the surface oxygen vacancy concentration increased, it was more likely that the subsurface O atoms transfer to the surface at zero H2 coverage (no H2 molecule on the surface), allowing the surface to maintain a stable Cu2O phase. However, when the H2 coverage was 0.25 monolayer (ML) (one H2 molecule every four surface Cu atoms), the presence of H atoms on the surface made the upward transfer of O atoms from the subsurface more difficult. The rate of consuming surface O atoms in the reduction reaction was greater than the rate of subsurface O atom transfer induced by the reduction reaction and the surface Cu2O phase could not be maintained stably. Through thermodynamic analysis, at high H2 concentration, the reaction between H2 and CuO was more likely to generate Cu, while at low H2 concentration, it was more likely to generate Cu2O. In summary, the valence state of Cu in the reaction process between CuO and H2 depended on the concentration of H2.

更新日期：2024-03-26

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