Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless,...Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.展开更多
The electrooxidation of CO on Ru (0001) and RuO2 (100) electrode surfaces were characterized by cyclic voltammetry, AES and RHEED. The CO adlayer was first partially oxidized at 0.8 V, which is controlled by the atta...The electrooxidation of CO on Ru (0001) and RuO2 (100) electrode surfaces were characterized by cyclic voltammetry, AES and RHEED. The CO adlayer was first partially oxidized at 0.8 V, which is controlled by the attack of oxygen species toward the Ru(0001) surface. The remaining CO adlayer oxidation at 0.55 V is related to the combination of CO molecules with oxygen species already located on the surface. In contrast, successive peaks on RuO2(100) at 0.4 V and 0.72 V are observed, which shows that CO molecules can directly react with two different lattice-oxygen on the surface to carbon dioxide.展开更多
采用模板法,以SiO2为模板,盐酸多巴胺(PDA)为碳源,通过SiO2构筑具有高度连通的三维多孔结构的氮掺杂中空介孔碳纳米材料(NMHCS),然后以NMHCS为载体,通过简单的预沉淀法将钌负载在碳球表面,制备具有钌负载的氮掺杂中空介孔碳纳米材料电...采用模板法,以SiO2为模板,盐酸多巴胺(PDA)为碳源,通过SiO2构筑具有高度连通的三维多孔结构的氮掺杂中空介孔碳纳米材料(NMHCS),然后以NMHCS为载体,通过简单的预沉淀法将钌负载在碳球表面,制备具有钌负载的氮掺杂中空介孔碳纳米材料电催化剂(Ru/NMHCS),并利用氧气进一步氧化得到Ru/RuO2异质结构电催化剂材料。该异质结构的纳米催化剂材料对析氧反应(OER)表现出显著的电催化活性,电流密度在10 m A·cm^(-2)处的过电位为270 mV,明显优于基准贵金属催化剂RuO2。为贵金属电催化剂的制备提供实验技术参考。展开更多
基金supported by the National Key R&D Program of China(2020YFB1505802)the Ministry of Science and Technology of China(2017YFA0208200,2016YFA0204100)+4 种基金the National Natural Science Foundation of China(22025108,U21A20327,and22121001)China Postdoctoral Science Foundation(2020M682083)Guangdong Provincial Natural Science Fund for Distinguished Young Scholars(2021B1515020081)Start-up Support from Xiamen University and the Guangzhou Key Laboratory of Low Dimensional Materials and Energy Storage Devices(20195010002)。
文摘Ru has recently been regarded as a promising catalyst for hydrogen oxidation reaction(HOR) and hydrogen evolution reaction(HER) due to its similar binding energy towards *H but lower price compared to Pt.Nevertheless, the quest of high-efficiency Ru-based catalysts for HOR and HER is driven by the current disadvantages including low activity and unsatisfactory stability. Herein, we have fabricated and engineered two-dimensional(2D) Ru-based snow-like nanosheets with Ru/Ru O2interface(Ru/Ru O2SNSs)via a post-annealing treatment. Detailed characterizations and theoretical calculations indicate that the interfacial synergy, which is dependent on the temperature for annealing, can alter the hydrogen binding energy(HBE) and hydroxide binding energy(OHBE), as a result of the enhanced HOR and HER performance. Impressively, the optimal Ru/RuO_(2) SNSs display a mass activity of 9.13 A mgRu^(–1) at an overpotential of 50 m V in 0.1 mol L^(–1) KOH for HOR, which is 65, 304, and 21 times higher than those of Ru SNSs(0.14 A mg_(Ru)^(–1)), RuO_(2) SNSs(0.03 A mg_(Ru)^(–1)), and commercial Pt/C(0.43 A mg_(Ru)^(–1)), respectively.Moreover, Ru/RuO_(2) SNSs display improved HER activity with a low overpotential of 20.2 m V for achieving10 m A cm^(-2)in 1 mol L^(–1)KOH. This work not only provides an efficient catalyst for HOR and HER, but also promotes fundamental research on the fabrication and modification of catalysts in heterogeneous catalysis.
文摘The electrooxidation of CO on Ru (0001) and RuO2 (100) electrode surfaces were characterized by cyclic voltammetry, AES and RHEED. The CO adlayer was first partially oxidized at 0.8 V, which is controlled by the attack of oxygen species toward the Ru(0001) surface. The remaining CO adlayer oxidation at 0.55 V is related to the combination of CO molecules with oxygen species already located on the surface. In contrast, successive peaks on RuO2(100) at 0.4 V and 0.72 V are observed, which shows that CO molecules can directly react with two different lattice-oxygen on the surface to carbon dioxide.
文摘采用模板法,以SiO2为模板,盐酸多巴胺(PDA)为碳源,通过SiO2构筑具有高度连通的三维多孔结构的氮掺杂中空介孔碳纳米材料(NMHCS),然后以NMHCS为载体,通过简单的预沉淀法将钌负载在碳球表面,制备具有钌负载的氮掺杂中空介孔碳纳米材料电催化剂(Ru/NMHCS),并利用氧气进一步氧化得到Ru/RuO2异质结构电催化剂材料。该异质结构的纳米催化剂材料对析氧反应(OER)表现出显著的电催化活性,电流密度在10 m A·cm^(-2)处的过电位为270 mV,明显优于基准贵金属催化剂RuO2。为贵金属电催化剂的制备提供实验技术参考。
