JOURNAL OF CATALYSIS
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2023
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IF 7.3
Guangmin Ren,Zehui Zhao,Zizhen Li,Zisheng Zhang,Xiangchao Meng
Herein, we applied a rapid Joule heating method to form oxygen vacancies and further induced the deposition of Ru clusters onto BiVO 4 . The rapid Joule heating method fabricated oxygen vacancy on BiVO 4 , resulting in the formation of electron-rich active Ru sites and unsaturated V sites. The pristine BiVO 4 was almost no activity in photocatalytic ammonia synthesis. The photocatalytic production rate of ammonia was increased to 3.88 μmol g - 1 h -1 after the formation of oxygen vacancies, and further increased to 16.57 μmol g -1 h -1 with Ru clusters loaded on BiVO 4 . It was indicated that unsaturated V sites near the oxygen vacancy and Ru clusters might act as the reactive sites for N 2 adsorption and activation. And the strong metal-support interactions between Ru and BiVO 4 resulted in charge redistribution between Ru clusters and BiVO 4 supports, thus reducing energy barrier of the rate-determining step for the N 2 hydrogenation. Furthermore, DFT confirmed that associative alternating pathway was suitable for this process.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
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IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
研究领域:
材料科学
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电化学
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能源技术
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DOI
PubMed
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-11
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IF 17.694
Zhang Yudi,Arpino Kathryn E.,Yang Qun,Kikugawa Naoki,Sokolov Dmitry A.,Hicks Clifford W.,Liu Jian,Felser Claudia,Li Guowei
Despite the fruitful achievements in the development of hydrogen production catalysts with record-breaking performances, there is still a lack of durable catalysts that could work under large current densities (>1000 mA cm −2 ). Here, we investigated the catalytic behaviors of Sr 2 RuO 4 bulk single crystals. This crystal has demonstrated remarkable activities under the current density of 1000 mA cm −2 , which require overpotentials of 182 and 278 mV in 0.5 M H 2 SO 4 and 1 M KOH electrolytes, respectively. These materials are stable for 56 days of continuous testing at a high current density of above 1000 mA cm −2 and then under operating temperatures of 70 °C. The in-situ formation of ferromagnetic Ru clusters at the crystal surface is observed, endowing the single-crystal catalyst with low charge transfer resistance and high wettability for rapid gas bubble removal. These experiments exemplify the potential of designing HER catalysts that work under industrial-scale current density.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
Energy Storage Materials
·
2022
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IF 20.831
Xuecheng Cao,Chaohui Wei,Xiangjun Zheng,Kai Zeng,Xin Chen,Mark H. Rummeli,Peter Strasser,Ruizhi Yang
Lithium–oxygen (Li–O 2 ) batteries have attracted tremendous attention due to their high specific energy density . However, their sluggish conversion kinetics and detrimental parasitic reactions would deteriorate the lifespan of batteries. Herein, a combined density functional theory (DFT) calculation and experimental approach is carried out to design an efficient cathode electrocatalyst for Li–O 2 batteries. A self-supporting film of Ru clusters anchored on Magnéli phase Ti 4 O 7 enriched with oxygen vacancy (Ru/Ti 4 O 7 ) is fabricated upon electrospinning and carbothermal reduction. In such a synergistic configuration of Ru/Ti 4 O 7 hybrid film, the strong metal-support interaction (SMSI) between Ru and Ti 4 O 7 can improve the charge transfer at the interface and enhance the adsorption energy of intermediates, accelerating the reaction kinetics of the formation/decomposition of Li 2 O 2 . Benefitting from this SMSI, the electrochemical stability of Ru/Ti 4 O 7 over cycling is also enhanced. As a result, as-prepared Ru/Ti 4 O 7 cathodes could realize excellent electrochemical performance , including high specific capacity (11000 mAh g –1 ), low discharge/charge polarization (0.36 V), long lifespan (> 100 cycles) and superior rate capability. Furthermore, a flexible Li–O 2 pouch cell, constructed with as-fabricated Ru/Ti 4 O 7 film cathode, lithium foil anode and GPE , can exert an impressive areal capacity of 5 mAh cm –2 with a low voltage gap of 0.82 V in ambient air. This work suggests that the activity of catalysts can be significantly enhanced with interfacial modification, offering an efficient approach for rational designing of electrocatalysts for use in Li–air batteries and beyond.
研究领域:
材料科学
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能源科学
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DOI
高影响因子
ACS Catalysis
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2022
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IF 13.7
Xilun Zhang,Lin Liu,Anan Wu,Junfa Zhu,Rui Si,Jianping Guo,Ruting Chen,Qike Jiang,Xiaohua Ju,Ji Feng,Zhitao Xiong,Teng He,Ping Chen
Metal-oxide-supported Ru catalysts, typically in the form of Ru particles dispersed on oxides, have emerged as the most promising catalysts for the ammonia synthesis reaction. Generally, Ru particles are regarded as catalytically active components and are mainly responsible for the formation of ammonia during ammonia synthesis. Here we show that subnano Ru clusters on Sm2O3 (Ru/Sm2O3) favor the formation of surface hydride (Sm–H) species under reaction conditions, which can trigger the activation of Ru clusters in the ammonia synthesis reaction. The synergy of surface hydride species and Ru clusters boosts the activity relative to Ru clusters alone and affords ammonia yields as high as 90.1–100% of the thermodynamic equilibrium value at 400 °C. Mechanistic studies and theoretical calculations reveal that Sm–H species can not only work in synergy with Ru clusters to reduce the energy barrier for nitrogen dissociation, but also directly participate in the formation of ammonia on the Ru clusters. The discovery of the synergy role of surface hydride species can deepen the molecular-level understanding of the ammonia synthesis reaction process, which will eventually help to rationally design efficient oxide-supported metal catalysts in the heterogeneous catalysis process where hydrogen is involved.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Lulu Chen,Bowen Lu,Juan Zhang,Renbing Wu,Yanhui Guo
Cobalt boride which is an active bifunctional water splitting catalyst in alkaline media shows poor activity in neutral media. We found that trace ruthenium (Ru) cluster deposition (80 μg·cm −2 ) on cobalt boride by simple wet chemical reduction method can dramatically improve both its hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) activity in neutral solution. The electron transfer from Co-B to Ru may result in the easier water dissociation step so as to facilitate the catalytic process. The resulting Ru@Co-B/Ni binder-free electrode could supply 10 mA cm −2 at overpotentials of 56 mV for HER and 280 mV for OER in 0.5 M phosphate buffer electrolyte. This work proposed a fruitful approach to advance the water splitting performance of transition metal boride in neutral media.
研究领域:
材料科学
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电化学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
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2022
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IF 8.047
Xilun Zhang,Lin Liu,Jiemin Wang,Xiaohua Ju,Rui Si,Ji Feng,Jianping Guo,Ping Chen
To exploit the ammonia as a carrier for sustainable energy, development of efficient catalysts is highly desired. Oxide supported Ru catalysts have been widely studied in ammonia synthesis for their superior catalytic performances under mild conditions. Here, sub-nanometer Ru clusters on La 2 O 3 (Ru clusters/La 2 O 3 ) catalyst has been synthesized and exhibits superior catalytic performance in ammonia synthesis under mild conditions. Multiple characterizations results reveal that surface La-H species, in situ generated on the surface of catalyst, can significantly boost the activity of Ru clusters/La 2 O 3 catalyst in ammonia synthesis. Detailed mechanistic studies demonstrate that the active La-H species on the La 2 O 3 can not only promote activation and dissociation of nitrogen molecules but also directly involve in ammonia synthesis reaction process via a La-H species-mediated reaction pathway. This work promotes molecular level understanding the active sites and reaction mechanism under real reaction conditions, and will also offer opportunity for guiding the design of efficient Ru-based catalysts for ammonia synthesis.
研究领域:
催化化学
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材料科学
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能源化学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xiang Li,Kelei Huang,Xiangchao Meng
The design of efficient electrocatalysts for hydrogen evolution reaction (HER) suitable for industrial applications remains a challenging task. In this work, Ru clusters were loaded onto WO 3 which were grown on carbon nanotubes (WRu/C-JH) using a rapid Joule heating method. The crystal phases of WO 3 was transformed, and abundant active sites were exposed during the rapid heating and cooling process. All these modifications contributed to the greatly improved electrocatalytic activity in HER. As tested, in 1 M KOH, it only required an overpotential of 22 mV to reach 10 mA cm −2 and 401 mV to reach a high current density of 1 A cm −2 on WRu/C-JH. Moreover, WRu/C-JH demonstrated excellent stability at 500 mA cm −2 for 100 h. Furthermore, a two-electrode system was constructed to assess overall water splitting performance of WRu/C-JH. This system was capable of reaching 100 mA cm −2 at a low voltage of 1.94 V. The mechanism of the enhancement in HER for as-prepared sample was also deeply discussed.
研究领域:
材料科学
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电催化
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产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Yao Xiao,Wengang Liu,Zhou Zhang,Jian Liu
Modulating the size and dispersion of metal particles is highly desirable in nanocatalysis. Herein highly dispersed ruthenium clusters confined in nitrogen-doped carbon (RuNC) were synthesized by a one-pot pyrolysis of Ru(phen) 3 organometallic compounds and glucose. The size of the Ru clusters was finely controlled at a cluster level (1.7 nm) to expose more catalytic active sites. The interaction between the Ru clusters and N species not only facilitated the uniform dispersion, but also prevented the aggregation of Ru clusters. This cluster-level RuNC manifested extraordinary catalytic performance towards the hydrogen evolution reaction (HER) and was comparable to or even better than a commercial Pt/C catalyst in basic and acidic media, respectively. Moreover, based on density functional theory (DFT) calculations, it was demonstrated that the N dopants in the carbon framework efficiently tailored the charge density distribution of the Ru centres and promoted the adsorption of H* on the catalyst, thus contributing to the high catalytic activity.
研究领域:
材料科学
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催化化学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Hengjun Gai,Xiaofeng Liu,Bingxiao Feng,Chaojie Gai,Tingting Huang,Meng Xiao,Hongbing Song
Ammonia nitrogen wastewater is the most abundant and widely distributed wastewater. In this work, a highly dispersed heterogeneous metal catalyst Ru@TiO 2 was successfully fabricated by a one-pot method for the catalytic wet air oxidation (CWAO) of ammonia. These catalysts were characterized by different techniques, indicating that Ru clusters were dispersed uniformly on the TiO 2 surface, and some Ru atoms were embedded in the TiO 2 framework. This structure can afford excellent catalytic performance, such as 0.5%Ru@TiO 2 catalyst offers a 95.5% conversion under the condition of 2 MPa at 190 °C in 6 h without adding alkali. Ammonia concentration can be reduced from 200 ppm to less than 10 ppm to meet emission standards. And the selectivity of ammonia oxidation products can be adjusted and controlled according to the reaction conditions. Besides, the kinetics and mechanism of CWAO of ammonia were studied, which provided a theoretical basis for its industrial application.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2024
·Vol. 155
·期 1
·1-10
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IF 2.3
Wang Shipeng,Sang Longrun,Zhang Feiyan,Li Yongcheng,Xu Benhua,Zhang Peng,Liu Bingxin,Wang Yunsi
Enhancing the performance of ruthenium (Ru)-based electrocatalysts for the alkaline hydrogen evolution reaction (HER) presents a significant challenge. Herein, titanium dioxide nanowire arrays decorated with ruthenium clusters were grown on carbon cloth (Ru-TiO 2 NWAs/CC) via a two-step hydrothermal method. The nanowire array structure increases the surface area of the substrate, allowing for more Ru clusters to be decorated, thereby improving catalytic activity. The resulting Ru 3 –TiO 2 NWAs/CC catalyst exhibits prominent HER performance in 1.0 M KOH with overpotentials of 61 at 10 mA cm −2 and a Tafel slope of only 47.4 mV dec −1 . Furthermore, it maintains outstanding stability under alkaline conditions for more than 10 h. The Ru clusters decoration enhances the TiO 2 /CC kinetic, more active sites were exposed on nanowires of the surface and accelerated electron transport, thus reducing the charge transfer barrier. After the electrochemical test, the morphology and structure of Ru 3 –TiO 2 /CC remained largely unchanged, and the valence states of the elements remained stable. This work paves the road to exploiting highly active and cost-efficient electrocatalysts for alkaline hydrogen evolution. Graphical
研究领域:
材料科学
·
电化学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2023
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IF 4.6
Tiantian Sun,Xinlin Wang,Zhiyao Duan,Qiong Zhang,Yingxiu Zhao,Guang-Rui Xu,Wei Wang,Lei Wang
Efficient and low-cost electrocatalysts for the hydrogen evolution reaction (HER) are required for producing hydrogen energy through water splitting. Carbon materials as HER catalyst supports are explored widely since the strong metal–support interactions are generally believed to be active and stable toward HER. Herein, we report N-doped porous carbon materials as novel substrates to stabilize the cluster metal sites through the Ru(III) polyamine complexes, which play an important role not only in efficient electron transfer but also in the increasing utilization of metallic active sites. Meanwhile, due to the strong metal–support interactions driven by Ru(III) polyamine complexes, the obtained Ru cluster with a mass loading of 3% on N-doped porous carbon nanoplates (Ru cluster@NCs) exhibits robust stability for HER at a constant voltage, proving to be a promising candidate catalyst for HER. Density functional theory calculations further indicate that the Gibbs free energy (ΔG) of adsorbed H* of Ru cluster@NCs is much closer to zero compared to Ru@(10%)NCs and Pt/C(20%), thus Ru cluster@NCs facilitate the HER process.
研究领域:
材料科学
·
催化化学
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产品关联
DOI
PubMed
高影响因子
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