CHINESE JOURNAL OF CATALYSIS
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2022
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IF 12.92
Liujing Yang,Chuanqi Cheng,Xun Zhang,Cheng Tang,Kun Du,Yuanyuan Yang,Shan-Cheng Shen,Shi-Long Xu,Peng-Fei Yin,Hai-Wei Liang,Tao Ling
Electrocatalytic reduction of nitrogen into ammonia (NH 3 ) is a highly attractive but challenging route for NH 3 production. We propose to realize a synergetic work of multi reaction sites to overcome the limitation of sustainable NH 3 production. Herein, using ruthenium-sulfur-carbon (Ru-S-C) catalyst as a prototype, we show that the Ru/S dual-site cooperates to catalyse eletrocatalytic nitrogen reduction reaction (eNRR) at ambient conditions. With the combination of theoretical calculations, in situ Raman spectroscopy, and experimental observation, we demonstrate that such Ru/S dual-site cooperation greatly facilitates the activation and first protonation of N 2 in the rate-determining step of eNRR. As a result, Ru-S-C catalyst exhibits significantly enhanced eNRR performance compared with the routine Ru-N-C catalyst via a single-site catalytic mechanism. We anticipate that our specifically designed dual-site collaborative catalytic mechanism will open up a new way to offers new opportunities for advancing sustainable NH 3 production.
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高影响因子
Nanoscale
·
2022
·Vol. 14
·期 42
·15724-15734
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IF 8.307
Shaohua Chai,Shuangde Li,Le Zhang,Guijun Fan,Linfeng Nie,Xin Zhou,Wuxinchen Yang,Weiman Li,Yunfa Chen
The regulation of oxygen vacancies and Ru species using metal–organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO2 and Ru/N-TiO2 catalysts were synthesized by the pyrolysis of MIL-125 and NH2-MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at ∼290 °C over Ru/M-TiO2 and Ru/N-TiO2 catalysts, while Ru/N-TiO2 showed quite less monochloromethane (MCM) and higher CO2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO2, compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO2. Additionally, Ru/N-TiO2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts.
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FUEL
·
2022
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IF 8.035
Zhuojie Zhong,Junxuan Li,Minyin Jian,Riyang Shu,Zhipeng Tian,Chao Wang,Ying Chen,Ning Shi,Yanxue Wu
Hydrodeoxygenation (HDO) reaction is a necessary refinery process for lignin-derived phenolic compounds to be used as high quality liquid fuels. Catalyst morphology makes a big difference on the HDO performance through changing the properties of metal site and acid site, while the catalytic mechanism is still not very clear. In this work, four kinds of Ru/TiO 2 catalysts with different morphology were prepared by photochemical method and all of them achieved a high Ru metal dispersion. A series of catalyst characterizations were carried out, including XRD, BET, SEM, TEM, H 2 -TPD and NH 3 -TPD, in order to explore the crystal structure, surface property, Ru metal dispersion, hydrogen adsorption capacity as well as acid properties. Results showed that Ru/TNP catalyst possessed a large surface area, an abundance of medium strength acid sites and a good hydrogen adsorption capacity. The HDO performances on lignin-derived phenolic compounds were also compared, in which Ru/TNP catalyst presented the best HDO performance. The guaiacol conversion and the selectivity of cyclohexane product were both close to 100 % at 250 °C under 1 MPa hydrogen pressure. Moreover, the content of hydrocarbons increased from 11.1 % to 60.8 % in the lignin-oil upgrading process.
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Inorganic Chemistry Frontiers
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2022
·Vol. 9
·期 15
·3885-3897
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IF 7.779
Kefeng Wang,Bin Li,Jingxiao Ren,Wenxia Chen,Jinhai Cui,Wei Wei,Peng Qu
Water splitting by electricity is believed to be a promising approach to obtain high-purity H2 on a large scale. Highly efficient electrocatalysts are of great importance for the electrocatalytic hydrogen evolution reaction (HER). Herein, we designed a highly efficient electrocatalyst (Ru@Ni3S2) for the HER by immersing Ni3S2 nanorod arrays into a RuCl3 aqueous solution. The obtained Ru@Ni3S2 with an increased electrochemical surface area and a decreased charge-transfer resistance demonstrates an enhanced electrocatalytic performance toward the HER in alkaline media, suggested by an overpotential of −19.8 mV to achieve a current density of 10 mA cm−2 and a Tafel slope of 33.2 mV dec−1. Both the in situ formed Ru nanoparticles and the adsorbed Ru3+ ions are responsible for the electrocatalytic hydrogen evolution reaction. Density functional theory (DFT) calculations reveal that the enhanced electrocatalytic HER activity of Ru@Ni3S2 compared with pure Ru can be ascribed to the lowered water dissociation energy barrier as well as the more favorable adsorption energy for the H intermediate (H*). During the long-term stability test, the adsorbed Ru3+ on the Ni3S2 nanorods would be converted to Ru(OH)3, leading to attenuated electrocatalytic activity. This drawback can be overcome by further surface modification with polyaniline (PANI). The obtained PANI–Ru@Ni3S2 exhibits a comparable catalytic HER activity to Ru@Ni3S2 but an extraordinary stability with continuous electrolysis at a current density of 20 mA cm−2 for 35 hours. Our design strategy here for synthesizing the Ru@Ni3S2 hybrid and effectively improving the stability of Ru-based catalysts could be extended to develop other noble metal/transition metal sulfides for practical water electrolysis and other applications.
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Chemistry-An Asian Journal
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2022
·Vol. 17
·期 17
·e202200449
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IF 4.839
Mingpu Jia,Ling Shen,Ge Tian,Susana I. Córdoba de Torresi,Mark D. Symes,Xiao-Yu Yang
Graphical The spatial junction in hierarchical confined CoNi/Ru@C has been synthesized, and its directional effect of electron transfer cascade can greatly promote the electrocatalytic hydrogen evolution in alkaline water/seawater. Exploiting directional electron transfer cascades could lead to high-performance electrocatalysts for processes such as the hydrogen evolution reaction, but realising such systems is difficult. Herein, a hierarchical confined material (CoNi/Ru@C) is presented, which provides a suitable spatial junction to enable directional electron transfer, giving superior hydrogen evolution in alkaline water/seawater.
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高影响因子
Energy & Environmental Materials
·
2022
·Vol. 6
·期 5
·e12418
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IF 13.443
Xiaobing Bao,Yuzhuo Chen,Shanjun Mao,Yong Wang,Yong Yang,Yutong Gong
The surface properties of catalysts determine the intrinsic activity and adaptability. Ruthenium is regarded as a potential candidate to substitute platinum for water electrolysis due to the low cost and analogous electronic structures while it suffers from severe dissolution and stability problems. Herein, the modification of Ru/C with atomically dispersed cobalt atoms is achieved via a simple thermal doping method. The newly formed amorphous shell with Ru-Co sites on the Ru/C catalyst improved the hydrogen evolution reaction activity and stability significantly. Impressively, the obtained Co 1 Ru@Ru/CN x catalyst exhibited an overpotential as low as 30 mV at 10 mA cm −2 in an alkaline medium, which is among the best HER catalysts reported so far. The oxygen oxophile Co prevents the fast oxidation and dissolution of Ru species, ensuring outstanding long-term durability up to 70 h. Theoretical calculations reveal that the Ru-Co coordination acts as a more active site for water dissociation than the Ru-Ru. Meanwhile, the “Ru-Co shell/Ru core” structures show high adaptability for the reaction conditions. This simple doping strategy offers prospects for scalable preparation of highly active electrocatalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Li Ji,Leheng Zhang,Huiyi Yang,Shan Liang,Junkang Pan,Yikui Zou,Shijia Li,Qinglan Li,Suqing Zhao
In view of the current public health hazards of food-borne pathogens, it is urgent to develop a rapid detection method with high sensitivity, good specificity and operational convenience, as well as to determine an effective sterilization strategy. Herein, versatile gold-ruthenium nanocomposites modified with antibody ( [email protected] Ncs) have been constructed for the sensitive detection of Salmonella typhimurium (S. typhimurium) via the lateral flow immunochromatographic assay (LFIA). [email protected] Ncs based LFIA exhibited a wide detection range from 2.9 × 10 6 CFU/mL to 2.9 × 10 11 CFU/mL with the limit of detection of 9.8 × 10 4 CFU/mL for S. typhimurium, and displayed excellent specificity. In addition, [email protected] Ncs irradiated with 808 nm (500 mW/cm 2 ) near-infrared light (NIR) had a significant antibacterial effect within only 5 min, attributed to its high photothermal conversion efficiency of 54.14%. Therefore, both sensitive detection of S. typhimurium and effective NIR-triggered photothermal sterilization were achieved by using versatile [email protected] Ncs, showing great prospects in the field of pathogen detection and treatment.
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ACS Nano
·
2022
·
IF 18.027
Qirui Liang,Qizhen Li,Lei Xie,Hui Zeng,Shan Zhou,Yanan Huang,Miao Yan,Xin Zhang,Tianyi Liu,Jie Zeng,Kang Liang,Osamu Terasaki,Dongyuan Zhao,Lei Jiang,Biao Kong
Hydrogen evolution reaction (HER) through water splitting is a potential technology to realize the sustainable production of hydrogen, yet the tardy water dissociation and costly Pt-based catalysts inhibit its development. Here, a trapping–bonding strategy is proposed to realize the superassembly of surface-enriched Ru nanoclusters on a phytic acid modified nitrogen-doped carbon framework (denoted as NCPO-Ru NCs). The modified framework has a high affinity to metal cations and can trap plenty of Ru ions. The trapped Ru ions are mainly distributed on the surface of the framework and can form Ru nanoclusters at 50 °C with the synergistic effect of vacancies and phosphate groups. By adjusting the content of phytic acid, surface-enriched Ru nanoclusters with adjustable distribution and densities can be obtained. Benefiting from the adequate exposure of the active sites and dense distribution of ultrasmall Ru nanoclusters, the obtained NCPO-Ru NCs catalyst can effectively drive HER in alkaline electrolytes and show an activity (at overpotential of 50 mV) about 14.3 and 9.6 times higher than that of commercial Ru/C and Pt/C catalysts, respectively. Furthermore, the great performance in solar to hydrogen generation through water splitting provides more flexibility for wide applications of NCPO-Ru NCs.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Fangjun Shao,Xiaojian Wang,Zijiang Zhao,Zhongzhe Wei,Xing Zhong,Zihao Yao,Shenwei Deng,Shibin Wang,Hong Wang,Aiyuan Li,Jianguo Wang
One-pot cascade transformations are environmentally friendly and are used to prepare complex organic molecules. However, chemselectivity is hard to control during the tandem reaction of imines. Herein, a Cu nanoparticle-decorated Ru cluster catalyst (Cu6Ru1.5/C-SiO2), with an average size of 2.1 nm, was designed and synthesized by impregnation and galvanic replacement. The synergistic effect of the Ru cluster and Cu nanoparticles caused Cu6Ru1.5/C-SiO2 to carry more Lewis acid active sites and constituted a unique catalyst surface. Then, the hydrogenation of nitrobenzene and reductive amination of benzaldehyde were effectively performed during a one-pot cascade transformation on the surface of the catalyst. Finally, N-benzylidene aniline (imine) was prepared smoothly by nitrobenzene and benzaldehyde with 96.3% selectivity in this catalytic system. This work provides a general and powerful strategy to optimize the catalytic performance, which can be scalable to other catalytic systems.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Wenlei Gu,An Pei,Shiyi Zhang,Feifei Jiang,Yanyan Jia,Qizhen Qin,Ruian Du,Zhengjian Li,Renfeng Liu,Yongcai Qiu,Keyou Yan,Yun Zhao,Cheng Liang,Guangxu Chen
The development of single-atom catalysts with effective interfaces for biomass conversion is a promising but challenging research area. In this study, a Ru1/CoOx catalyst was successfully fabricated with the impregnation method, which featured Ru single atoms on a cobalt oxide substrate. The Ru1/CoOx catalyst showed superior performance in the selective electrooxidation of 5-hydroxymethylfurfural (HMF) to produce 2,5-furandicarboxylic acid (FDCA), a high value-added product. The introduction of Ru single atoms with an ultralow loading of ∼0.5 wt % was revealed to accelerate the electroredox of Co2+/Co3+/Co4+ and improve the intrinsic activity of the CoOx substrate with an FDCA selectivity of 76.5%, which is better than that of the pristine CoOx electrocatalysts (62.7%). The interfacial synergistic effect of the Ru1/CoOx interface clarified that Ru single atoms can enhance the adsorption of HMF at the Ru1/CoOx interface, which promoted the rate-determining step of the selective C–H bond activation for FDCA production. This finding provides valuable insights into the rational design of single-atom catalysts with functional interfaces for biomass upgrading.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2021
·
IF 8.128
Jianmei Cen,Pei Kang Shen,Yanfei Zeng
Herein, a novel Ru-doped bimetal phosphide (Ru-NiCoP) heterostructure electrocatalyst on Ni foam is successfully synthesized through a multi-step hydrothermal reaction , ion exchange, and phosphorization method for efficient overall water splitting in alkaline media. The doping of Ru and P can effectively optimize the electronic structure and expose more active sites. The unique 3D interconnected nanowires not only ensures the uniform distribution of Ru coupled with NiCoP, but also endows the Ru-NiCoP/NF with the large ECSA, the fast electron transport and the favorable reaction kinetics attributes. Benefiting from the compositional and structural advantages, Ru-NiCoP/NF catalyst exhibits significantly enhanced catalytic activities along with excellent stability, only needing 32.3 mV at 10 mA cm −2 for HER and 233.8 mV at 50 mA cm −2 for OER . In particular, when Ru-NiCoP/NF is employed as both cathode and anode electrodes, a small voltage of 1.50 V is required to reach 30 mA cm −2 for overall water splitting with an impressive stability. This study provides an alternative strategy on the design and development of high performance catalysts for overall water splitting and other energy conversion fields.
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ACS Materials Letters
·
2021
·
IF 8.312
Rui Tang,Zhijie Zhu,Chaoran Li,Mengqi Xiao,Zhiyi Wu,Dake Zhang,Chengcheng Zhang,Yi Xiao,Mingyu Chu,Alexander Genest,Günther Rupprechter,Liang Zhang,Xiaohong Zhang,Le He
Cascade catalysis of reverse water gas shift (RWGS) and well-established CO hydrogenation holds promise for the conversion of greenhouse gas CO2 and renewable H2 into liquid hydrocarbons and methanol under mild conditions. However, it remains a big challenge to develop low-temperature RWGS catalysts with high activity, selectivity, and stability. Here, we report the design of an efficient RWGS catalyst by encapsulating ruthenium clusters with the size of 1 nm inside hollow silica shells. The spatially confined structure prevents the sintering of Ru clusters while the permeable silica layer allows the diffusion of gaseous reactants and products. This catalyst with reduced particle sizes not only inherits the excellent activity of Ru in CO2 hydrogenation reactions but also exhibits nearly 100% CO selectivity and superior stability at 200–500 °C. The ability to selectively produce CO from CO2 at relatively low temperatures paves the way for the production of value-added fuels from CO2 and renewable H2.
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