• 主题
高级搜索  >
历史搜索 清空历史
首页> 美国卫生研究院文献>Advanced Science >Interfacial Engineering of SeO Ligands on Tellurium Featuring Synergistic Functionalities of Bond Activation and Chemical States Buffering toward Electrocatalytic Conversion of Nitrogen to Ammonia
【2h】

Interfacial Engineering of SeO Ligands on Tellurium Featuring Synergistic Functionalities of Bond Activation and Chemical States Buffering toward Electrocatalytic Conversion of Nitrogen to Ammonia

机译：碲上SeO配体的界面工程具有键活化和化学态缓冲的协同功能可实现氮到氨的电催化转化

代理获取
本网站仅为用户提供外文OA文献查询和代理获取服务，本网站没有原文。下单后我们将采用程序或人工为您竭诚获取高质量的原文，但由于OA文献来源多样且变更频繁，仍可能出现获取不到、文献不完整或与标题不符等情况，如果获取不到我们将提供退款服务。请知悉。
页面导航
  • 摘要
  • 著录项
  • 相似文献
  • 相关主题

摘要

Ammonia (NH3) production from electrochemical nitrogen (N2) reduction reaction (NRR) under ambient conditions represents a sustainable alternative to the traditional Haber–Bosch process. However, the conventional electrocatalytic NRR process often suffers from low selectivity (competition with the hydrogen evolution reaction (HER)) and electron transfer bottleneck for efficient activation and dissociation. Herein, a strategy to simultaneously promote selectivity and activity through dual‐incorporation of Se and O elements onto the shell of HER‐inactive Te nanorods is reported. It is theoretically and experimentally verified that the exposure of lone‐pair electrons in the TeO2 shell of Se, O dual‐doped Te nanorods can maximize orbits overlap between N2 and Te for N‐N bond activation via π‐backdonation interactions. Further, the Gibbs free energy change indicates that the Lewis‐basic anchor ‐SeO ligand with strong electron‐donating characteristics serves as an electron reservoir and is capable of buffering the oxidation state variation of Te, thereby improving the thermodynamics of desorption of the intermediates in the N2‐to‐NH3 conversion process. As expected, a high faradaic efficiency of 24.56% and NH3 yield rate of ≈21.54 µg h−1 mg−1 are obtained under a low overpotential of ≈0.30 V versus reversible hydrogen electrode in an aqueous electrolyte under ambient conditions.
机译：在环境条件下，通过电化学氮（N2）还原反应（NRR）生产氨（NH3）代表了传统Haber-Bosch工艺的可持续替代方案。然而，常规的电催化NRR工艺通常具有低选择性（与氢释放反应（HER）竞争）和有效转移和有效电子转移的瓶颈。本文报道了一种通过将Se和O元素双重掺入HER失活的Te纳米棒壳中来同时提高选择性和活性的策略。理论上和实验上都证明，在Se，O双掺杂的Te纳米棒的TeO2壳层中孤对电子的暴露可以通过π返配相互作用使N2和Te之间的轨道重叠最大化，从而激活N‐N键。吉布斯自由能的变化表明，具有强电子给体特性的路易斯碱锚-SeO配体可作为电子储库，并能够缓冲Te的氧化态变化，从而提高了中间体的解吸热力学。 N2到NH3的转换过程。正如预期的那样，在约0.30 V的低过电位相对于可逆的情况下，可以获得高达24.56％的法拉第效率和NH3产率≈21.54µg h -1 mg -1 氢电极在环境条件下在水性电解质中。

著录项

相似文献

  • 外文文献
  • 中文文献
  • 专利
代理获取

客服邮箱：kefu@zhangqiaokeyan.com

京公网安备：11010802029741号 ICP备案号：京ICP备15016152号-6 六维联合信息科技 (北京) 有限公司©版权所有

  • 客服微信

  • 服务号