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Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction

文献类型:期刊论文

作者Tao, HC; Choi, C; Ding, LX; Jiang, Z; Hang, ZS; Jia, MW; Fan, Q; Gao, YN; Wang, HH; Robertson, AW
刊名CHEM
出版日期2019
卷号5期号:1页码:204—214
ISSN号2451-9294
关键词ELECTROCHEMICAL AMMONIA-SYNTHESIS ATMOSPHERIC-PRESSURE HYDROGENATION N-2 TEMPERATURE CATALYSTS WATER
DOI10.1016/j.chempr.2018.10.007
文献子类期刊论文
英文摘要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 N-2 selectively to NH3, affording an NH3 formation rate of 3.665 mg(NH3) h(-1) mg(Ru)(-1) 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 N-2 adsorption. We envision that optimization of ZrO2 loading could further facilitate electroreduction of N-2 at both high NH3 synthesis rate and faradic efficiency.
语种英语
源URL[http://ir.sinap.ac.cn/handle/331007/31725]  
专题上海应用物理研究所_中科院上海应用物理研究所2011-2017年
作者单位1.Korea Adv Inst Sci & Technol, Grad Sch Energy Environm Water & Sustainabil, Daejeon 34141, South Korea;
2.Beijing Univ Chem Technol, State Key Lab Organ Inorgan Composites, Beijing 100029, Peoples R China;
3.South China Univ Technol, Sch Chem & Chem Engn, Guangzhou 510640, Guangdong, Peoples R China;
4.Chinese Acad Sci, Shanghai Inst Appl Phys, Shanghai Synchrotron Radiat Facil, Shanghai 201204, Peoples R China;
5.Univ Oxford, Dept Mat, Oxford OX1 3PH, England;
6.Korea Adv Inst Sci & Technol, Dept Chem & Biomol Engn, Daejeon 34141, South Korea
推荐引用方式
GB/T 7714
Tao, HC,Choi, C,Ding, LX,et al. Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction[J]. CHEM,2019,5(1):204—214.
APA Tao, HC.,Choi, C.,Ding, LX.,Jiang, Z.,Hang, ZS.,...&Sun, ZY.(2019).Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction.CHEM,5(1),204—214.
MLA Tao, HC,et al."Nitrogen Fixation by Ru Single-Atom Electrocatalytic Reduction".CHEM 5.1(2019):204—214.

入库方式: OAI收割

来源:上海应用物理研究所

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