当前位置: X-MOL 学术Chem › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction
Chem ( IF 19.1 ) Pub Date : 2018-11-08 , DOI: 10.1016/j.chempr.2018.10.007
Hengcong Tao , Changhyeok Choi , Liang-Xin Ding , Zheng Jiang , Zishan Han , Mingwen Jia , Qun Fan , Yunnan Gao , Haihui Wang , Alex W. Robertson , Song Hong , Yousung Jung , Shizhen Liu , Zhenyu Sun

Nitrogen fixation under ambient conditions remains a significant challenge. Here, we report nitrogen fixation by Ru single-atom electrocatalytic reduction at room temperature and pressure. In contrast to Ru nanoparticles, single Ru sites supported on N-doped porous carbon greatly promoted electroreduction of aqueous N2 selectively to NH3, affording an NH3 formation rate of 3.665 mgNH3h1mgRu1 at −0.21 V versus the reversible hydrogen electrode. Importantly, the addition of ZrO2 was found to significantly suppress the competitive hydrogen evolution reaction. An NH3 faradic efficiency of about 21% was achieved at a low overpotential (0.17 V), surpassing many other reported catalysts. Experiments combined with density functional theory calculations showed that the Ru sites with oxygen vacancies were major active centers that permitted stabilization of *NNH, destabilization of *H, and enhanced N2 adsorption. We envision that optimization of ZrO2 loading could further facilitate electroreduction of N2 at both high NH3 synthesis rate and faradic efficiency.



中文翻译:

Ru单原子电催化还原固氮

在环境条件下固氮仍然是一项重大挑战。在这里,我们报告在室温和压力下通过Ru单原子电催化还原进行固氮。与Ru纳米颗粒相比,负载在N掺杂的多孔碳上的单个Ru位置极大地促进了N 2选择性地电还原为NH 3,从而使NH 3的形成速率为3.665GñH3H-1个G-1个相对于可逆氢电极为-0.21V。重要的是,发现添加ZrO 2可以显着抑制竞争性的析氢反应。在低过电势(0.17 V)时,NH 3法拉第效率达到了约21%,超过了许多其他报道的催化剂。与密度泛函理论计算相结合的实验表明,具有氧空位的Ru位是主要的活性中心,可以使* NNH稳定,* H不稳定和增强N 2吸附。我们预见到ZrO 2负载的优化可以进一步促进N 2在高NH 3合成速率和法拉第效率下的电还原。

更新日期:2018-11-08
down
wechat
bug