ACS Applied Materials & Interfaces
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2020
·
IF 8.758
Xuzhuo Sun,Xuyun Gao,Jing Chen,Xin Wang,Haixia Chang,Bo Li,Dengmeng Song,Jun Li,Haisheng Li,Ning Wang
Nanostructuring and metal–support interactions have been explored as effective methods to improve the electrocatalytic activity in heterogeneous catalysis. In this study, we have fabricated ultrasmall Ru nanoparticles (NPs) dispersed on S-doped graphene (denoted as Ru/S-rGO) by a facile “one-pot” procedure. The experimental results indicated that both the S doping and moderate degree of oxidization of GO can induce the formation and high dispersion of the ultrasmall Ru NPs with larger electrochemically active surface areas for exposing more active sites. Metal–support interaction between S-doped graphene and Ru NPs was observed from the X-ray photoelectron spectroscopy and electronic charge-difference studies. It resulted in the decrease in the electron density of Ru, which facilitated electron release from H2O and H–OH bond breakage. The results of density functional theory calculation confirmed that the S-dopants could reduce the energy barrier for breaking the H–OH bond to accelerate water dissociation during the alkaline hydrogen evolution reaction (HER). At a current density 20 mA cm–2, the lowest overpotential of 14 mV, superior to that of Pt/C in alkaline solution, was observed for Ru/S-rGO-24. The observed lowest value of overpotential was because of the ultrasmall size, high dispersion, and metal–support interaction. This work provides a simple and effective method in designing advanced electrocatalysts for the HER in an alkaline electrolyte.
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ACS Catalysis
·
2020
·
IF 12.35
Xiuyun Wang,Lingling Li,Zhongpu Fang,Yongfan Zhang,Jun Ni,Bingyu Lin,Lirong Zheng,Chak-tong Au,Lilong Jiang
The industrial synthesis of NH3 using Fe- or Ru-based catalysts usually requires harsh reaction conditions. It is desirable to develop catalysts that perform well at low temperature and pressure (250–400 °C, <2 MPa). The main challenge of low-temperature NH3 synthesis is the dissociation of the extremely stable N≡N triple bond. Herein, we report the design of homogeneous single-atom Ru centers on an H-ZMS-5 (HZ) support with the Ru atoms individually anchored in the micropores of HZ, effectively boosting NH3 synthesis under mild conditions via an associative pathway. Synchrotron-based near-edge X-ray absorption fine structure (NEXAFS) and in situ DRIFTS analyses show that ═N– groups are the primary intermediates, and DFT calculations further show that, unlike Ru nanoclusters, the cooperation of a single Ru atom and hydrogen species in HZ leads to N2 hydrogenation rather than direct N2 dissociation, and the indirect N–N bond dissociation occurs much more easily via the formation of the NHNH3* intermediate; the energy barrier for breaking the N–N bond keeps falling from 2.90 eV for *N2 to 0.04 eV for *NHNH3, showing that N2 hydrogenation is an effective way for sharp weakening of N–N bonds. Moreover, the rate-determining step is shifted from the dissociation of the N≡N triple bond to the formation of *N2H2. As a consequence, the single-atom 0.2 wt % Ru/H-ZSM-5 catalyst shows the highest NH3 synthesis rate per gram of Ru (1.26 molNH3 gRu–1 h–1 at 300 °C and 1 MPa) among the Ru-based catalysts ever reported.
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Materials
·
2020
·Vol. 13
·期 18
·4026
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IF 3.057
Shasha Zhang,Wenxin Ji,Ning Feng,Liping Lan,Yuanyuan Li,Yulong Ma
In this study, a Rh(I)/Ru(III) catalyst with a bimetallic space structure was designed and synthesized. The interaction between the metals of the bimetallic catalyst and the structure of the bridged dimer can effectively reduce the steric hindrance effect and help speed up the reaction rate while ensuring the stability of the catalyst. X-ray photoelectron spectroscopy (XPS) results show that rhodium accepts electrons from chlorine, thereby increasing the electron-rich nature of rhodium and improving the catalytic activity. This promotes the nucleophilic reaction of the catalyst with methyl iodide and reduces the reaction energy barrier. The methanol carbonylation performance of the Rh/Ru catalyst was evaluated, and the results show that the conversion rate of methyl acetate and the yield of acetic acid are 96.0% under certain conditions. Furthermore, during the catalysis, no precipitate is formed and the amount of water is greatly reduced. It can be seen that the catalyst has good stability and activity.Keywords:carbonylation;acetic acid;bimetallic catalyst
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JOURNAL OF SOLID STATE CHEMISTRY
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2020
·
IF 2.726
Haodong Tang,Yao Wang,Wujian Zhang,Zongjian Liu,Lichun Li,Wenfeng Han,Ying Li
SmCeO x composite oxide with Sm 3+ occupying Ce 4+ site in CeO 2 crystal lattice , prepared via citric acid complexation method, was loaded with 2 w% Ru by impregnation method and the as-prepared catalyst was then evaluated for ammonia decomposition. The results show that the partial substitution of Ce 4+ by Sm 3+ produces a positive effect on the catalyst performance and SmCeO x supported Ru exhibits a much higher low-temperature catalytic activity for ammonia decomposition compared with other supports such as Sm 2 O 3 , CeO 2 , and a physical mixture of Sm 2 O 3 and CeO 2 . For example, the ammonia conversion is increased from 54.6% to 74.9% at a temperature of 400 °C and a space velocity of 3900 ml/g cat ·h when CeO 2 is replaced by Sm 0.4 Ce 0.6 O 1.8 . TEM and CO chemisorption investigations reveal that the excellent performance of Ru/SmCeO x catalyst is related to its high Ru dispersion. The results of BET, EPR and H 2 -TPR suggest that the partial substitution of Ce 4+ with Sm 3+ may induce the formation of oxygen vacancies and the high Ru dispersion can be attributed to the presence of large amount of single-electron trapped oxygen vacancies on the surface of SmCeO x , which have a strong interaction with Ru and thus Ru preferentially occupies the oxygen vacancies. This experimental observation is also supported by the DFT calculation result that Ru species adsorbed on the oxygen vacancy has a low adsorption energy .
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JOURNAL OF ALLOYS AND COMPOUNDS
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2020
·
IF 4.65
Mingrui Wei,Shuo Huang,Yun Wang,Yihui Liu,Yunfei He,Chao Wang,Lan Yang
Ru-doped Co 3 O 4 (Ru x Co 3-x O 4 , 0.1 ≤ x ≤ 0.3) catalysts are prepared by co-precipitation method. The prepared powders are characterized by X-ray diffraction (XRD), scanning electron microscope (SEM), energy dispersive spectrometer (EDS), transmission electron microscope (TEM), inductively coupled plasma-optical emission spectrometry (ICP-OES), Brunauer-Emmett-Teller (BET) test and X-ray photoelectron spectroscopy (XPS). These characterization methods confirm that the crystal structure of Ru x Co 3-x O 4 is consistent with that of Co 3 O 4 , and the catalyst powders are in the form of nanoparticles with an average particle diameter of about 20 nm. The electrochemical performances of the catalysts are evaluated by cyclic voltammograms and linear sweep voltammograms in 0.1 M KOH solution. When x = 0.2, Ru x Co 3-x O 4 shows the best electrochemical performances with the onset potential (E onset ) at 0.88 V, the half-wave potential (E 1/2 ) at 0.77 V and the limited current density at 4.41 mA cm −2 . The oxygen reduction reaction for Ru x Co 3-x O 4 mainly follows four-electron pathway with the electron transfer number at about 3.5. Furthermore, Ru 0.2 Co 2.8 O 4 has greater stability and anti-methanol property than Pt/C. These results revealed that Ru x Co 3-x O 4 is an oxygen reduction catalyst with high performance and low cost.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2021
·
IF 5.816
Wenkai Huang,Fuhua Xu,Xiang Liu
Sodium borohydride has been widely regarded as a promising hydrogen carrier owing to its greatly hydrogen storing capability (10.8 wt%), high weight density and excellent stability in alkaline solutions. Herein, we first design and synthesize a series of bimetallic M-Ru/C nanocomposites (including Fe–Ru/C, Co–Ru/C, Ni–Ru/C and Cu–Ru/C), via simply alloying of commercial Ru/C with nonprecious metal, for superior H 2 evolution from the NaBH 4 hydrolysis. The result exhibits that H 2 generation is synergetically improved by alloying Ru/C with Co or Ni, while it is hindered by alloying Ru/C with Fe or Cu. Indeed, Co–Ru/C presents the highest efficient catalytic activity for H 2 generation, with the TOF of 117.69 mol(H 2 )·mol Ru −1 ·min −1 , whereas Ru/C is only 57.08 mol(H 2 )·mol Ru −1 ·min −1 . In addition, the TOF of Co–Ru/C reaches to 436.51 mol(H 2 )·mol Ru −1 ·min −1 (96.7 L(H 2 )·g Ru −1 ·min −1 ) in the presence of NaOH.
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NEW JOURNAL OF CHEMISTRY
·
2021
·Vol. 45
·期 32
·14406-14413
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IF 3.591
Yubo Liu,Guoqiang Ding,Guoping Zhao,Haohao She,Yulei Zhu,Yong Yang
Combining glucose dehydration and the subsequent hydrogenation in one pot is a preferable approach for process development as such a method allows in situ generation of the reactive intermediate to undergo further reaction without extra energy-intensive separation. Herein, phosphotungstic acid and various types of titania (anatase, rutile, P25) supported Ru-based catalysts were considered as the dehydration and hydrogenation catalysts, respectively. Modulating the different reactant media (N2, H2), various products were obtained with GBL–H2O as the solvent. A considerable yield (42%) of levulinic acid (LA) and γ-valerolactone (GVL) (40%) were obtained in nitrogen and subsequent hydrogen. Ru/TiO2 (rutile) was the favorable hydrogenation catalyst among the three types of Ru/TiO2. Meanwhile, a certain amount of sorbitol (36%) was obtained in pure hydrogen. The hydrogenation of glucose is more likely to occur than the glucose dehydration. The physicochemical properties of the catalysts were characterized by XRD, BET, TPR, STEM and in situ CO/FT-IR, and the results show that well-dispersed Ru particles are located on the rutile crystallites, which facilitated the hydrogenation of LA. A strong metal support interaction (SMSI) was responsible for the various microstructure properties and the different hydrogenation reactivity. This work allows a better understanding of the reaction paths of glucose conversion.
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Catalysis Science & Technology
·
2020
·Vol. 10
·期 5
·1336-1342
·
IF 5.721
Ziqi Zhang,Kaida Yao,Linchuan Cong,Zhuochen Yu,Lina Qu,Weimin Huang
Ammonia is one of the most important agricultural fertilizers and renewable energy carriers, and is also one of the most highly produced inorganic compounds in the world. The traditional industrial ammonia synthesis mainly uses the Haber–Bosch method, which consumes a large amount of fossil fuels and emits a lot of greenhouse gas. Thus, a more environmentally friendly method is needed for the production of ammonia. In this paper, we present a new electrocatalyst to produce NH3 under ambient conditions, which was obtained via the carbonization of Ru-dispersed ZIF-8. As a result, the catalyst could achieve a maximum NH3 production rate of about 16.68 μgNH3 h−1 mgcat.−1 at −0.4 V (vs. RHE) and a faradaic efficiency of 14.23% at −0.3 V (vs. RHE) at room temperature and ambient pressure in 0.1 M KOH. Also, the loading of Ru is only 16 wt%. Thus, this work provides a feasible method to design highly dispersed noble metal electrocatalysts for the nitrogen reduction reaction (NRR).
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Inorganic Chemistry Frontiers
·
2019
·Vol. 6
·期 6
·1382-1387
·
IF 5.934
Yuanmeng Zhao,Guixiang Mao,Chaozhang Huang,Ping Cai,Gongzhen Cheng,Wei Luo
Searching for highly efficient and stable electrocatalysts applied for the hydrogen evolution reaction (HER) in an alkaline solution is highly desirable, but still remains a challenge due to the sluggish water dissociation kinetics. Herein, in this work, ultrafine Ru nanoparticle (NP) decorated WSe2 nanosheets have been successfully prepared by a colloidal synthetic approach. Benefiting from the interfacial synergy effect between WSe2 nanosheets and Ru NPs, the rate-determining water dissociation step for the alkaline HER and the subsequent hydrogen generation step are speeded up. As expected, the resultant Ru–WSe2 hybrid with 1.93 wt% Ru loading exhibits excellent catalytic performance for HER media, with an overpotential of 87 mV to achieve a current density of 10 mA cm−2, and superior long-term stability.
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ANALYTICAL SCIENCES
·
2019
·Vol. 35
·期 6
·639-644
·
IF 1.618
Shan Xueling,Pan Yuting,Chen Xiaohui,Wang Wenchang,Chen Zhidong
A novel electrochemiluminescence (ECL) sensor for detection of brilliant blue FCF (BB) has been developed using Ru@ Zn-MOF/nafion modified GCE (glass carbon electrode) in this research. Different from conventional method for usage of Ru(bpy) 3 2+ in solution-phase, Ru(bpy) 3 2+ here was immobilized on a zinc-metal-organic-framework (Zn-MOF). After adding BB, a significant quenching phenomenon of ECL intensity was observed. The behavior of BB on the quenching effect of Ru(bpy) 3 2+ /Zn-MOF in different conditions was investigated thoroughly and the detection limit was achieved to 2.5 × 10 −8 M in an optimized condition. Furthermore, the interference of some conventional ions and amino acids to the detection of BB was also investigated. Additionally, the composite showed a good effect on the detection of BB in commercial samples. The proposed sensor provided a promising platform for food safety analysis, environmental monitoring and clinical testing.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Yueling Cao,Hepeng Zhang,Kangkai Liu,Qiuyu Zhang,Kai-Jie Chen
A synergistic effect normally exists in bimetallic catalysts, which can greatly improve the catalytic performance in comparison with monometallic catalysts. However, the N-doped carbon-supported bimetallic catalysts, especially for noble-based bimetallic catalysts prepared by one-pot pyrolysis at high temperatures are scarcely reported. Herein, a novel sustainable Ru–MoOx bimetallic catalyst was successfully prepared by one-pot pyrolysis of biowaste (chitin) and metal salts, which exhibited great improvement in catalytic activity and could be stable up to 5 cycles for the direct hydrogenation of furfural (FAL) to tetrahydrofurfuryl alcohol (THFA). On the basis of series of catalyst characterizations, it was found that there was a strong interaction between Ru and MoOx particles, behaving as the main contributor to the enhanced catalytic performance.
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Journal of CO2 Utilization
·
2019
·
IF 5.189
Shanshan Chai,Yong Men,Jinguo Wang,Shuang Liu,Qiaoling Song,Wei An,Gunther Kolb
Catalytic reduction of CO 2 to methane has been recognized as one of the most important strategic reactions to produce highly valuable chemicals and for storage of renewable energy (power-to-gas). This study demonstrates a crystal facet-dependent catalytic reduction of CO 2 to CH 4 on ruthenium nanoparticles deposited over TiO 2 nanocrystal with exposed (001) and (101) facets. Compared with TiO 2 (101) nanocrystal with the same Ru loading, Ru nanoparticles supported by TiO 2 (001) exhibited a highly enhanced CO 2 conversion rate and significantly improved methanation reactivity, along with a considerable durability. The physicochemical properties of the samples were characterized by HR-TEM, XRD, BET, FT-IR, UV–vis, Raman, ICP, and temperature-programmed reaction with CO 2 , and CO 2 + H 2 . In view of the difference in catalytic activity and the physicochemical properties of the supported Ru/TiO 2 catalysts, the results uncovered that the nature of the catalyst support of Ru/TiO 2 strongly affected the dispersion of Ru species and the synergistic effect between Ru and underlying TiO 2 supporting materials due to the strong metal-support interaction, and thus affected their capability to activate CO 2 and determined the catalytic activity for CO 2 methanation. Our work demonstrated the important role of the exposed crystal facets of the underlying support and the resulting Ru particle which had a large effect on CO 2 methanation.
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