ChemCatChem
·
2020
·Vol. 12
·期 20
·5149-5155
·
IF 4.853
Suli Liu,Xueqin Mu,Pengxia Ji,Yun Lv,Lei Wang,Quan Zhou,Changyun Chen,Shichun Mu
Graphical Decorating nanorods : We demonstrate the first metal-phosphides-metal system consisting of Ru and FeCoP, which forms unique CoFeP@Ru nanorod using a simple one-pot synthetic method. Due to its optimal dual cation decorating effects, improved conductivity and rod-like morphology, this catalyst shows superior electro-catalytic HER and OER performances, which are superior to those of some recently reported phosphides and close to that of commercial catalysts. Interfacial engineering and defect modulation can provide abundant active sites for catalysts to further boost the catalysis process. In this work, we develop a strategy to grow multi-heterogeneous cobalt phosphide (CoP) nanorods with rich interfaces and defects along the one-dimensional (1D) nanostructure by dual incorporation of Fe and Ru (CoFeP@Ru). Such a catalyst exhibits high activity and stability towards the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with overpotentials of only 38 mV in 0.5 M H 2 SO 4 and 48 mV in 1.0 M KOH for HER, and an overpotential of 340 mV in 0.1 M KOH for OER at 10 mA cm −2 . Finally, as the bifunctional catalyst, an alkali electrolyzer is assembled and delivers at a low cell voltage, with almost 100 % Faradaic efficiency. Our experimental results demonstrate that Fe incorporation can disturb or even break the periodic structure of cobalt phosphides, causing a redistribution of the electronic structure and electron density of activity sites, while Ru can significantly enhance the catalytic kinetics, as well as electrochemical and mechanical stability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Shaoxian Song,Song Wu,Yating He,Yiwen Zhang,Guangyin Fan,Yan Long,Shuyan Song
Developing a straightforward and general strategy to regulate the surface microenvironment of a carbon matrix enriched with N/B motifs for efficient atomic utilization and electronic state of metal sites in bifunctional hydrogen production via ammonia-borane hydrolysis (ABH) and water electrolysis is a persistent challenge. Herein, we present a simple, green, and universal approach to fabricate B/N co-doped porous carbons using ammonia-borane (AB) as a triple functional agent, eliminating the need for hazardous and explosive functional agents and complicated procedures. The pyrolysis of AB induces the regulation of the surface microenvironment of the carbon matrix, leading to the formation of abundant surface functional groups, defects, and pore structures. This regulation enhances the efficiency of atom utilization and the electronic state of the active component, resulting in improved bifunctional hydrogen evolution. Among the catalysts, B/N co-doped vulcan carbon (Ru/BNC) with 2.1 wt% Ru loading demonstrates the highest performance in catalytic hydrogen production from ABH, achieving an ultrahigh turnover frequency of 1854 min −1 (depending on the dispersion of Ru). Furthermore, this catalyst shows remarkable electrochemical activity for hydrogen evolution in alkaline water electrolysis with a low overpotential of 31 mV at 10 mA cm −2 . The present study provides a simple, green, and universal method to regulate the surface microenvironment of various carbons with B/N modulators, thereby adjusting the atomic utilization and electronic state of active metals for enhanced bifunctional hydrogen evolution.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Yujie Xie,Bianyong Lian,Shuqi Deng,Qingqu Lin,Kaili Wang,Yun Zheng,Zewen Zhuang,Yao Liu,Kaian Sun,Wei Yan,Jiujun Zhang
CO and H 2 S poisoning of Pt-based catalysts for hydrogen oxidation reaction (HOR) stands as one of the long-standing hindrances to the widespread commercialization of proton exchange membrane fuel cells. In this paper, a Ru/Ti 4 O 7 catalyst is successfully synthesized by the microwave-thermal method. This Ru/Ti 4 O 7 catalyst shows a much higher noble metal mass activity than those of commercial PtRu/C and conventional Ru/C catalysts. The performance of the Ru/Ti 4 O 7 catalyst under the exist of CO or H 2 S shows insignificant current decay, which is far superior to commercial PtRu/C and Pt/C catalysts. In this Ru/Ti 4 O 7 catalyst, the electron transfer between Ru and Ti to form d-p orbital hybridization is considered to be responsible for the favorable catalytic HOR performance and the corresponding CO and H 2 S tolerance. The interaction mechanism formed by electron transfer may open a promising way for the subsequent development of anti-poisoning catalysts for PEM fuel cell hydrogen oxidation reaction.
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高影响因子
MOLECULES
·
2024
·Vol. 29
·期 10
·2255
·
IF 4.2
Yan Cui,Zequan Zeng,Yaqin Hou,Shuang Ma,Wenzhong Shen,Zhanggen Huang
Noble metals have become a research hotspot for the oxidation of light alkanes due to their low ignition temperature and easy activation of C-H; however, sintering and a high price limit their industrial applications. The preparation of effective and low-noble-metal catalysts still presents profound challenges. Herein, we describe how a Ru@CoMn2O4spinel catalyst was synthesized via Ru in situ doping to promote the activity of propane oxidation. Ru@CoMn2O4exhibited much higher catalytic activity than CoMn2O4, achieving 90% propane conversion at 217 °C. H2-TPR, O2-TPD, and XPS were used to evaluate the catalyst adsorption/lattice oxygen activity and the adsorption and catalytic oxidation capacity of propane. It could be concluded that Ru promoted synergistic interactions between cobalt and manganese, leading to electron transfer from the highly electronegative Ru to Co2+and Mn3+. Compared with CoMn2O4, 0.1% Ru@CoMn2O4, with a higher quantity of lattice oxygen and oxygen mobility, possessed a stronger capability of reducibility, which was the main reason for the significant increase in the activity of Ru@CoMn2O4. In addition, intermediates of the reaction between adsorbed propane and lattice oxygen on the catalyst were monitored by in situ DRIFTS. This work highlights a new strategy for the design of a low-noble-metal catalyst for the efficient oxidation of propane.
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RSC Advances
·
2016
·Vol. 6
·期 49
·42994-42999
·
IF 3.289
Zonggang Mu,Lei Jiao,Qin Wei,He Li
Nobel metal nanoparticles have attracted intense attentions in biological immunoassay due to the inhereted good catalytic activity. In this study, a new kind of nanocomposite of ternary Pt@Pd@Ru nanodendrite-decorated graphene oxide (GO–Pt@Pd@Ru) was prepared as a signal label for ultrasensitive detection of carcinoembryonic antigen (CEA). With a sandwich type immunoassay, the established electrochemical immunosensor showed highly sensitive detection performance towards CEA in a linear range (0.1 pg mL−1 to 9 ng mL−1) with an ultralow detection limit of 0.05 pg mL−1. The enhancing detection performance could be attributed to: ternary Pt@Pd@Ru nanodendrites have exhibited superior electrochemical reduction activity towards H2O2, then GO–Pt@Pd@Ru can combine all generated electrochemical reduction current towards H2O2 by the decorated Pt@Pd@Ru nanodendrites, which can significantly amplify the detection signal.
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ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Xun Li,Hui Hu,Tian Tan,Mengjing Sun,Yuwen Bao,Zhongbing Huang,Sohail Muhammad,Xiaohong Xia,Yun Gao
Detection of leaks of flammable methane (CH4) gas in a timely manner can mitigate health, safety, and environmental risks. Zinc oxide (ZnO), a polar semiconductor with controllable surface defects, is a promising material for gas sensing. In this study, Ag–Ru co-doped into self-assembled ZnO nanorod arrays (ZnO NRs) was prepared by a one-step hydrothermal method. The Ag–Ru co-doped sample shows a good hydrophobic property as a result of its particular microstructure, which results in high humidity resistance. In addition, oxygen vacancy density significantly increased after Ag–Ru co-doping. Density functional theory (DFT) calculations revealed an exceptionally high charge density accumulated at the Ru sites and the formation of a localized strong electric field, which provides additional energy for the CH4 reaction with •O2– at the surface at room temperature. Optimized AgRu0.025–ZnO demonstrated an outstanding CH4 sensing performance, with a limit of detection (LOD) as low as 2.24 ppm under free-heat and free-light conditions. These findings suggest that introducing defects into the ZnO lattice, such as oxygen vacancies and localized ions, offers a promising approach to improving the gas sensing performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Dianzhi Zhang,Haiming Gong,Tao Liu,Jiaguo Yu,Panyong Kuang
Chlorine evolution reaction (CER) is crucial for industrial-scale production of high-purity Cl 2 . Despite the development of classical dimensionally stable anodes to enhance CER efficiency, the competitive oxygen evolution reaction (OER) remains a barrier to achieving high Cl 2 selectivity. Herein, a binder-free electrode, Ru nanoparticles (NPs)-decorated NiMoO 4 nanorod arrays (NRAs) supported on Ti foam (Ru-NiMoO 4 /Ti), was designed for active CER in saturated NaCl solution (pH = 2). The Ru-NiMoO 4 /Ti electrode exhibits a low overpotential of 20 mV at 10 mA cm −2 current density, a high Cl 2 selectivity exceeding 90%, and robust durability for 90h operation. The marked difference in Tafel slopes between CER and OER indicates the high Cl 2 selectivity and superior reaction kinetics of Ru-NiMoO 4 /Ti electrode. Further studies reveal a strong metal-support interaction (SMSI) between Ru and NiMoO 4 , facilitating electron transfer through the Ru–O bridge bond and increasing the Ru 3d–Cl 2p antibonding orbital occupancy, which eventually results in weakened Ru–Cl bonding, promoted Cl desorption, and enhanced Cl 2 evolution. Our findings provide new insights into developing electrodes with enhanced CER performance through antibonding orbital occupancy engineering.
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高影响因子
APPLIED SURFACE SCIENCE
·
2024
·
IF 6.3
Min Chen,Longgang Liu,Xueyan Chen,Xiaoxiao Qin,Kunlin Li,Jianghao Zhang,Xiaolei Bao,Lingjuan Ma,Changbin Zhang
The influence of metal particle size over heterogeneous catalysts on the catalytic performance has always been an interesting subject due to its significance from both fundamental and practical perspectives. In this work, we regulated the synthesis of TiO 2 by the hydrolysis of different titanium precursors, and as-prepared TiO 2 supports were employed to load Ru with impregnation method. Interestingly, we synthesized three Ru-TiO 2 catalysts with different Ru particle sizes of 1.1, 2.9 and 5.2 nm. The Ru-TiO 2 catalysts were next tested for CO 2 hydrogenation reaction, the results show that the medium Ru particles on TiO 2 exhibited the best CO 2 methanation activity. Based on the characterizations, we observed that the medium Ru particles exhibited the best redox properties compared with small and large Ru particles, which was beneficial to the H 2 dissociation; in addition, the medium Ru particles exhibited a moderate ability to activate CO 2 , resulting in the most favorable formation and decomposition of bidentate bicarbonate. Consequently, the Ru-TiO 2 catalyst with medium Ru particles showed the highest activity for CO 2 methanation. This study provides a new method to prepare Ru-TiO 2 catalysts with different Ru sizes and also presents an understanding of Ru particle size effects on CO 2 hydrogenation.
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Qiaohong Su,Qingcui Liu,Pengyue Wang,Juan Ding,Jiulin Wang,Yudai Huang
High overpotential and low stability are major challenges for hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). Tuning the electronic structure of catalysts is regarded as a core strategy to enhance catalytic activity. Herein, we report CuO x /Cu nanorod skeleton supported Ru doped cobalt oxide/nitrogen-doped carbon nanocomposites (Ru-CoO/NC/CuO x /Cu, denoted as RCUF) as bifunctional catalysis. The one-dimensional/three-dimensional (1D/3D) nanostructure and defect-rich amorphous/crystalline phases of RCUF facilitates active site exposure and electron transport. Experimental characterization and density functional theory (DFT) calculation results indicate that Ru doping can optimize the electronic structure, which accelerates the water dissociation process and reduces the Gibbs free energy of the reaction intermediates. As expected, the optimal RCUF-900 exhibits low overpotential (25/205 mV at 10 mA cm −2 ) and high stability (100/100 h) for HER/OER. RCUF-900 has low voltage (1.54 V at 10 mA cm −2 ) and high stability (100 h) for overall water splitting. This work provides new insights into the design of advanced catalysts for overall water splitting.
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Nanoscale
·
2024
·
IF 5.8
Heyun Lin,Wenzhe Zhang,Huachen Shen,Hailing Yu,Yunlei An,Tiejun Lin,Liangshu Zhong
The catalytic behavior of CO hydrogenation can be modulated by metal–support interactions, while the role of the support remains elusive. Herein, we demonstrate that the presence of strong metal–support interactions (SMSI) depends strongly on the crystal phase of TiO2 (rutile or anatase) and the treatment conditions for the TiO2 support, which could critically control the activity and selectivity of Ru-based nanocatalysts for CO hydrogenation. High CO conversion and olefin selectivity were observed for Ru/rutile-TiO2 (Ru/r-TiO2), while catalysts supported by anatase (a-TiO2) showed almost no activity. Characterization confirmed that the SMSI effect could be neglected for Ru/r-TiO2, while it is dominant on Ru/a-TiO2 after reduction at 300 °C, resulting in the coverage of Ru nanoparticles by TiOx overlayers. Such SMSI could be suppressed by H2 treatment of the a-TiO2 support and the catalytic activity of the as-obtained Ru/a-TiO2(H2) can be greatly elevated from almost inactive to >50% CO conversion with >60% olefin selectivity. Further results indicated that the surface reducibility of the TiO2 support determines the SMSI state and catalytic performance of Ru/TiO2 in the CO hydrogenation reaction. This work offers an effective strategy to design efficient catalysts for the FTO reaction by regulating the crystal phase of the support.
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Journal of Materials Chemistry A
·
2024
·Vol. 12
·期 18
·10713-10725
·
IF 10.7
Xiaoling Ye,Wencheng Liu,Yan Lu,Xiaoxiao Zheng,Yijian Bi,Min Zheng,Lei Han,Benqing Liu,Yafei Ning,Syed Hassan Mujtaba Jafri,Xinyu Zhao,Shangming He,Shilin Zhang,Hu Li
Li–CO2 batteries have emerged as a potential candidate for next-generation energy storage devices due to their impressive theoretical energy density and potential for CO2 capture. However, the practical application of these batteries faces a challenge due to the sluggish CO2 reduction reaction kinetics and Li2CO3 decomposition at the cathode. Herein, graphene nanoribbons decorated with Ru nanoparticles (GNR/Ru) as cathode catalysts are reported, where dispersed Ru nanoparticles on conductive graphene networks are effective in catalyzing CO2 reduction and Li2CO3 decomposition. As a result, the cathode using GNR/Ru catalysts demonstrates a high discharge capacity of 11 470 mA h g−1 at 100 mA g−1 and exhibits excellent long-term stability (more than 1240 hours) with a low overpotential of 1.34 V at a fixed capacity of 500 mA h g−1. This study provides new insights for exploring high-performance cathodic catalysts.
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2024
·
IF 18.5
Jiahui Wang,Min Zhou,Rong Fu,Ju Ge,Wei Yang,Xufeng Hong,Congli Sun,Xiaobin Liao,Yan Zhao,Zhaoyang Wang
Electrocatalytic hydrogen evolution and (S 2− ) recycling present promising strategies for cost-effective hydrogen production and simultaneous removal of environmental pollutants. However, the advancement of this technology is hindered by the limited availability of affordable, efficient, and stable catalysts. Herein, the study synthesizes ultrafine ruthenium (Ru) nanoclusters on a substrate of iron molybdenum sulfide (FeMo-S) nanosheets, creating a new heterointerface catalyst (FeMo-S/Ru) for the hydrogen evolution reaction (HER) and sulfion oxidation reaction (SOR). Experimental and theoretical calculations suggest that strong electron interactions between Ru nanoclusters and FeMo-S substrate, optimizing *H adsorption and promoting HER activity on one side while facilitating the production and adsorption of sulfur intermediates on the other side, effectively catalyzing SOR. Additionally, the assembled electrocatalytic coupling system with FeMo-S/Ru displays an ultralow cell voltage of 0.57 V at 100 mA cm −2 , achieving high Faradaic efficiencies (>96%) for H 2 production, while also exhibiting remarkable durability over 1 month (838 h). This work paves the way for the development of highly efficient and durable supported catalysts, enabling energy-saving hydrogen production and environmentally friendly sulfion recycling.
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