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Highly efficient and selective nitrate electroreduction to ammonia catalyzed by molecular copper catalyst@Ti3C2Tx MXene
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2021-09-02 , DOI: 10.1039/d1ta06664a Lan-Xin Li 1 , Wu-Ji Sun 1 , Hao-Yu Zhang 1 , Jia-Liang Wei 1 , Shu-Xian Wang 1 , Jing-Hui He 1 , Na-Jun Li 1 , Qing-Feng Xu 1 , Dong-Yun Chen 1 , Hua Li 1 , Jian-Mei Lu 1
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2021-09-02 , DOI: 10.1039/d1ta06664a Lan-Xin Li 1 , Wu-Ji Sun 1 , Hao-Yu Zhang 1 , Jia-Liang Wei 1 , Shu-Xian Wang 1 , Jing-Hui He 1 , Na-Jun Li 1 , Qing-Feng Xu 1 , Dong-Yun Chen 1 , Hua Li 1 , Jian-Mei Lu 1
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The efficient electroreduction reaction of nitrate (NO3−RR) at low concentrations to ammonia is energetically favorable for ammonia production and environmentally essential to treat water contamination. Copper-based conjugated molecule electrocatalysts for the NO3−RR are advantageous in terms of their customizable Cu-coordinative micro-environment and facile preparation; however, they easily agglomerate due to their large π-conjugating system, which severely lowers the active site density and increases the internal resistance. This study demonstrates that Ti3C2Tx MXenes are promising supports to disperse and anchor a molecular catalyst (copper phthalocyanine, CuPc) to construct a CuPc@MXene electrocatalyst in order to significantly promote NO3−RR performance. 10% CuPc@MXene achieved higher ammonia selectivity (94.0%) and higher nitrate conversion (90.5%) compared to those of unsupported CuPc, and retained high ammonia selectivity (∼80%) after seven recycling tests. The combination of online differential electrochemical mass spectroscopy (DEMS) and density functional theory (DFT) calculations has showed that CuPc molecules are able to inhibit the hydrogen evolution reaction and effectively convert nitrate into ammonia through the ONH reaction pathway. The results showed that the MXene support is applicable to many metal phthalocyanines (MPcs, M = Fe, Co, Ni), demonstrating its potential in other electrochemical catalysis applications.
中文翻译：
分子铜催化剂@Ti3C2Tx MXene催化高效选择性硝酸盐电还原氨
低浓度硝酸盐 (NO 3 - RR)的有效电还原反应生成氨在能量上有利于氨的生产，并且对处理水污染具有环境重要性。用于NO 3 - RR的铜基共轭分子电催化剂在其可定制的Cu配位微环境和容易制备方面具有优势；然而，由于它们的大π共轭体系，它们很容易团聚，这严重降低了活性位点密度并增加了内阻。该研究表明 Ti 3 C 2 T xMXenes 是分散和锚定分子催化剂（铜酞菁，CuPc）以构建 CuPc@MXene 电催化剂以显着促进 NO 3 - 的有希望的载体RR 性能。与未负载的 CuPc 相比，10% CuPc@MXene 实现了更高的氨选择性（94.0%）和更高的硝酸盐转化率（90.5%），并在七次循环测试后保持了高氨选择性（~80%）。在线微分电化学质谱 (DEMS) 和密度泛函理论 (DFT) 计算的结合表明，CuPc 分子能够抑制析氢反应，并通过 ONH 反应途径有效地将硝酸盐转化为氨。结果表明，MXene 载体适用于许多金属酞菁（MPcs，M = Fe，Co，Ni），证明了其在其他电化学催化应用中的潜力。
更新日期：2021-09-24
中文翻译：
分子铜催化剂@Ti3C2Tx MXene催化高效选择性硝酸盐电还原氨
低浓度硝酸盐 (NO 3 - RR)的有效电还原反应生成氨在能量上有利于氨的生产，并且对处理水污染具有环境重要性。用于NO 3 - RR的铜基共轭分子电催化剂在其可定制的Cu配位微环境和容易制备方面具有优势；然而，由于它们的大π共轭体系，它们很容易团聚，这严重降低了活性位点密度并增加了内阻。该研究表明 Ti 3 C 2 T xMXenes 是分散和锚定分子催化剂（铜酞菁，CuPc）以构建 CuPc@MXene 电催化剂以显着促进 NO 3 - 的有希望的载体RR 性能。与未负载的 CuPc 相比，10% CuPc@MXene 实现了更高的氨选择性（94.0%）和更高的硝酸盐转化率（90.5%），并在七次循环测试后保持了高氨选择性（~80%）。在线微分电化学质谱 (DEMS) 和密度泛函理论 (DFT) 计算的结合表明，CuPc 分子能够抑制析氢反应，并通过 ONH 反应途径有效地将硝酸盐转化为氨。结果表明，MXene 载体适用于许多金属酞菁（MPcs，M = Fe，Co，Ni），证明了其在其他电化学催化应用中的潜力。
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