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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 |
DOI | 10.1016/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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