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Highly Selective Conversion of CH4 to High Value-Added C1 Oxygenates over Pd Loaded ZnTi-LDH
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-06-19 , DOI: 10.1002/aenm.202301118 Lei Fu 1 , Ruixue Zhang 1 , Jianlong Yang 1 , Jiale Shi 1 , Hai‐Ying Jiang 1 , Junwang Tang 2
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2023-06-19 , DOI: 10.1002/aenm.202301118 Lei Fu 1 , Ruixue Zhang 1 , Jianlong Yang 1 , Jiale Shi 1 , Hai‐Ying Jiang 1 , Junwang Tang 2
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The selective oxidation of methane to high value-added liquid oxygenated compounds under mild conditions is of great significance to promote the efficient utilization of the carbon source, but it also faces the dilemma of low activity and over-oxidation. Here, ZnTi-layered double hydroxides (LDH)-A200 photocatalysts with Pd loading are prepared to achieve efficient oxidation of methane, with O2 as an oxidant under ambient condition. The highest generation rate of C1 liquid products (methanol and formaldehyde) reaches 4924.47 µmol g−1 h−1 with a selectivity close to 100% over 0.5Pd-ZnTi-LDH-A200, which is 20 times higher than that of bare ZnTi-LDH-A200. The photochemical results show that the modified photocatalysts present much higher generation and separation efficiency of electron-hole pairs. In situ X–ray photoelectron spectroscopy indicates that Pd nanoparticles are the hole acceptor, which is beneficial to charge separation in the photocatalysis. Furthermore, electron spinresonance spectroscopy and temperature–programmed–desorption analysis prove that Pd loading is helpful to the adsorption of methane and oxygen on the surface of ZnTi-LDH-A200, promoting the production of reactive oxygen species and activation of methane. All these factors work together to promote the efficient conversion of CH4 to high value-added C1 oxygenates.
中文翻译：
通过负载 Pd 的 ZnTi-LDH 将 CH4 高度选择性转化为高附加值的 C1 含氧化合物
温和条件下甲烷选择性氧化为高附加值液态含氧化合物对于促进碳源的高效利用具有重要意义，但也面临着活性低和过度氧化的困境。本文制备了负载Pd的ZnTi层状双氢氧化物(LDH)-A200光催化剂，以在环境条件下以O 2作为氧化剂实现甲烷的有效氧化。C 1液体产物（甲醇和甲醛）最高生成率达到4924.47 µmol g −1 h −1与0.5Pd-ZnTi-LDH-A200相比，选择性接近100%，是裸ZnTi-LDH-A200的20倍。光化学结果表明，改性光催化剂具有更高的电子-空穴对的产生和分离效率。原位X射线光电子能谱表明Pd纳米颗粒是空穴受体，有利于光催化中的电荷分离。此外，电子自旋共振光谱和程序升温脱附分析证明，Pd负载有助于甲烷和氧气在ZnTi-LDH-A200表面的吸附，促进活性氧的产生和甲烷的活化。所有这些因素共同作用，促进CH 4高效转化为高附加值C 1充氧。
更新日期：2023-06-20
中文翻译：
通过负载 Pd 的 ZnTi-LDH 将 CH4 高度选择性转化为高附加值的 C1 含氧化合物
温和条件下甲烷选择性氧化为高附加值液态含氧化合物对于促进碳源的高效利用具有重要意义，但也面临着活性低和过度氧化的困境。本文制备了负载Pd的ZnTi层状双氢氧化物(LDH)-A200光催化剂，以在环境条件下以O 2作为氧化剂实现甲烷的有效氧化。C 1液体产物（甲醇和甲醛）最高生成率达到4924.47 µmol g −1 h −1与0.5Pd-ZnTi-LDH-A200相比，选择性接近100%，是裸ZnTi-LDH-A200的20倍。光化学结果表明，改性光催化剂具有更高的电子-空穴对的产生和分离效率。原位X射线光电子能谱表明Pd纳米颗粒是空穴受体，有利于光催化中的电荷分离。此外，电子自旋共振光谱和程序升温脱附分析证明，Pd负载有助于甲烷和氧气在ZnTi-LDH-A200表面的吸附，促进活性氧的产生和甲烷的活化。所有这些因素共同作用，促进CH 4高效转化为高附加值C 1充氧。
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