RENEWABLE ENERGY
·
2022
·
IF 8.634
Wei Lv,Xiaohong Hu,Yuting Zhu,Ying Xu,Shijun Liu,Peili Chen,Chenguang Wang,Longlong Ma
Herein, the catalysts of ruthenium and molybdenum oxide nanoparticles supported on activated carbon (AC) were synthesized by precursor stepwise impregnation and employed for the hydrodeoxygenation (HDO) of lignin oil. The XRD, TEM, XPS and NH 3 -TPD-MS result of RuMoO x /AC catalysts confirm that the method of loading molybdenum precursor before ruthenium precursor is advantageous for the MoO x and Ru nanoparticles high dispersion and the reduction of MoO x species enhance the amount of acidity of catalyst. Meanwhile, the reduction temperature of RuMoO x /AC-1-T catalysts could effectively regulate the MoO x species that determine the activity and product distribution of HDO. The conversion of aromatic monomers/dimers were up to 96% with high selectivity of hydrocarbon over RuMoO x /AC-1-350 catalyst at 160 °C and 30 bar H 2 . Which is attributed to the MoO 3 and Ru species possess the excellent activity of benzene ring deep hydrogenation, ether bond breaking and acid dehydration. The RuMoO x /AC-1-350 catalyst effectively converted lignin oil (from the depolymerization of cornstalk hydrolysis residue) into hydrocarbons (56.9 wt%) and cyclohexanol/ethers (18.7 wt%) under 280 °C and 3 bar H 2 . The durability of the RuMoO x /AC-1-350 catalyst for HDO of lignin oil was also investigated and showed that the RuMoO x /AC-1-350 catalyst had good stability, regenerability and repeatability.
✓ 已验证
DOI
高影响因子
Nature Communications
·
2022
·Vol. 13
·期 1
·1-10
·
IF 17.694
Zhou Jun,Gao Zhe,Xiang Guolei,Zhai Tianyu,Liu Zikai,Zhao Weixin,Liang Xin,Wang Leyu
Supports can widely affect or even dominate the catalytic activity, selectivity, and stability of metal nanoparticles through various metal-support interactions (MSIs). However, underlying principles have not been fully understood yet, because MSIs are influenced by the composition, size, and facet of both metals and supports. Using Ru/TiO 2 supported on rutile and anatase as model catalysts, we demonstrate that metal-support interfacial compatibility can critically control MSI modes and catalytic performances in CO 2 hydrogenation. Annealing Ru/rutile-TiO 2 in air can enhance CO 2 conversion to methane resulting from enhanced interfacial coupling driven by matched lattices of RuO x with rutile-TiO 2 ; annealing Ru/anatase-TiO 2 in air decreases CO 2 conversion and converts the product into CO owing to strong metal-support interaction (SMSI). Although rutile and anatase share the same chemical composition, we show that interfacial compatibility can basically modify metal-support coupling strength, catalyst morphology, surface atomic configuration, MSI mode, and catalytic performances of Ru/TiO 2 in heterogeneous catalysis.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2022
·
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.
✓ 已验证
产品关联
DOI
高影响因子
Nano Research
·
2023
·Vol. 16
·期 10
·12223-12229
·
IF 9.9
Li Rongxiang,Zeng Wei,Zhao Runyao,Zhao Yanfei,Wang Yuepeng,Zhang Fengtao,Tang Minhao,Wang Ying,Chang Xiaoqian,Wu Fengtian,Liu Zhimin
Production of fuel and chemicals from plastic waste is one of the effective ways to upcycle spent plastics, which is an interesting topic and of significance for green and sustainable development. Herein, we demonstrate a highly efficient catalyst, TiO 2 nanoparticle supported Ru nanocatalyst (Ru/TiO 2 ), for upcycling polyethylene terephthalate (PET) to alkanes in the presence of H 2 and water. Under the optimal conditions (200 °C, 60 bar H 2 , and small amount of H 2 O), PET could completely convert into alkanes, dominated with cyclohexane and methane. It was indicated that the strong interaction between the TiO 2 support and Ru nanoparticles made electrons flow from the TiO 2 support to the Ru nanoparticles, which thus rendered Ru/TiO 2 to have ability to simultaneously catalyze PET hydrolysis and intermediate hydrogenation. This work realizes the transformation of PET to alkanes, which provides a promising way to chemically upcycle PET.
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Jun Zhang,Chengyu Li,Haoran Yuan,Yong Chen
In the present study, Ru modified hierarchical zeolites x Ru-MZSM were developed for cellulose fast pyrolysis . Comprehensive catalyst characterizations including XRD , XPS , N 2 adsorption-desorption, Py-IR and so on, were performed to unveil the essential structural properties. The chemical modification and Ru decoration remarkably regulated the distribution of Brønsted/Lewis acid sites. The presence of RuO x species would supply abundant strong Lewis acid sites for participating catalytic cracking , dehydration, decarbonylation, decarboxylation, cyclization, aromatization, etc., in cooperation with Brønsted acid sites. In-situ generated active Ru 0 centers during cellulose pyrolysis might facilitate the proceeding of deoxygenation , hydride transfer, and dehydrogenation . Among the as-prepared catalysts screened, 2Ru-MZSM was much more efficient in aromatics production from cellulose fast pyrolysis compared to parent ZSM, wherein the total aromatics yield achieved 16.8% at temperature of 650 °C and heating rate of 10 °C/ms with corresponding E value as low as 23.40 kJ/mol. Also, plausible reaction mechanism for x Ru-MZSM involved cellulose fast pyrolysis was proposed in detail.
✓ 已验证
产品关联
DOI
高影响因子
Polymers
·
2023
·Vol. 15
·期 24
·4735
·
IF 5
Xiaofang Fu,Zhuohui Zhang,Zhenhu Cao,Alexandr Alexandrovich Rogachev,Maxim Anatolievich Yarmolenko,Tao Chen,Hongtao Cao,Hongliang Zhang
The metallo-supramolecular polymer (MSP) is considered one of the most promising electrodes for electrochromic devices due to its intrinsically stable redox properties. Nevertheless, despite extensive work focusing on improving the electrochromic and electrochemical properties of MSPs, little experimental evidence exists from in-depth investigations on the anion-induced electrochromism of MSPs. Herein, Ru-based metallo-supramolecular polymer (polyRu) films with excellent electrochromic performance were fabricated through a novel electrochemical deposition method, and the electrochromic mechanism was further understood. The polyRu films possess fast reaction kinetics with a short switching time of 4.0 s (colored) and 2.8 s (bleached) and highly reversible redox properties due to the resulting impacts on the capacitive behaviors (containing surface, near-surface and intercalation pseudo-capacitance) of the perchlorate ions in the electrochromic process. Moreover, the electrochromic degradation of the polyRu films is considered to stem from the numerous nanopores in the film induced by ClO4−transport and the exchange of counter anions from Cl−to ClO4−. In addition, a physical model, revealing the transport of conduction ions and the evolution of the structure and properties of the polyRu film during the electrochromic process, is presented. It is observed that the charge balance of Ru3+and Ru2+, achieved through the adsorption/desorption of ClO4−on the film, provides electrochromic and electrochemical reversibility to the polyRu film under positive/negative bias. Correspondingly, a transformation from polyRu·(Cl−)2nto polyRu·(ClO4−)x(Cl−)2n−xin the polyRu film is induced by a counter anion exchange from Cl−to ClO4−. Revealing the detailed perchlorate ion transfer kinetics and electrochromic mechanism in this film can offer new insights into the application of metallo-supramolecular polymers in electrochromic devices.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Tianfen Huang,Ruiyi Wang,Jin Zhang,Jiapei Wang,Hui Ge,Jun Ren,Zhanfeng Zheng
Graphitic carbon nitride (g-C 3 N 4 ) based materials has been widely used for catalytic CO 2 hydrogenation reaction. However, the catalytic activity is restricted due to the barren active sites and the weak ability to activate CO 2 for the traditional g-C 3 N 4 . We demonstrate here that cyano group modified g-C 3 N 4 supported Ru nanoparticles exhibits high activity and selectivity for CO 2 methanation. The introduction of cyano group promotes the formation of medium basic sites for enhanced CO 2 adsorption. Meanwhile, the formation of electron-rich Ru nanoparticles with the assistance of cyano group boosts the H 2 activation. The synergistic effect of cyano group and Ru nanoparticles improves catalytic performance up to 14 times. Characterizations prove that cyano group with electron-withdrawing properties influences the way of CO 2 adsorption via electron transfer and changes the CO 2 hydrogenation reaction pathway. This work provides a new insight into the switching of CO 2 hydrogenation pathway and enhanced catalytic activity via surface functional groups modification of g-C 3 N 4 based catalyst.
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2026
·
IF 18.1
Hu Yingjie,Long Yongde,Mao Baoguang,Yu Zeqiang,Zhao Linjie,Tang Cheng,Kou Ruitian,Sun Chaoyang,Hu Chuangang
The oxide path mechanism offers vision possibility from kinetics for the anodic oxygen evolution reaction, yet its universal activation remains elusive due to the difficulty of constructing globally appropriate interatomic distances. Here, we address this challenge in the integrated-screened Y 0.1 Ir 0.2 Ru 0.7 O x by precisely regulating the Ru-Ru 1 bond length and constructing locally ordered yet long-range disordered structures that dissipate lattice strain, thereby enabling homogeneous modulation of interatomic distances across the framework. In-situ infrared spectroscopy together with online mass spectrometry confirms that the catalyst consistently follows a universal pathway. Building on these structural and mechanistic advantages, the nanostructured catalyst achieves a low cell voltage of 1.75 V@3 A cm -2 with operational stability ( > 2800 h @ 3 A cm -2 , 0.0625 mV h -1 decay rate) in proton exchange membrane water electrolysis. This work establishes a generalizable framework for pervasive dual-site catalysis, providing a paradigm for next-generation water electrolysis anodes and beyond.
✓ 已验证
产品关联
DOI
高影响因子
ADVANCED MATERIALS
·
2026
·
IF 29.1
Linlin Hou,Ying Liu,Hongjie Cui,Ziying Qin,Muyao Liu,Lunqiao Xiong,Yong Chen,Haifeng Wang,Junwang Tang
Ammonia, as an emerging energy carrier, holds significant strategic importance in the transition of future energy systems. Although the Haber-Bosch process remains the dominant industrial route for ammonia synthesis, its high energy demand and substantial carbon emissions underscore the urgent need for sustainable alternatives. Herein, ruthenium (Ru) with an average particle size of 0.9 nm supported on BaTiO 3 is developed, which enables photon-phonon co-driven ammonia synthesis at low temperature and pressure. Photon-generated electrons effectively mitigate the H 2 poisoning effect and more importantly remarkably promote N 2 adsorption and dissociation on Ru sites, thereby working together with phonons to accelerate hydrogenation along the dissociative pathway. As a result, the ammonia synthesis rate reaches 746.6 mmol g Ru −1 h −1 at 350 °C under ambient pressure and 2269 mmol g Ru −1 h −1 under 2 MPa via photon-phonon co-driven catalysis, representing a very low apparent activation energy of 24 kJ mol −1 and a 51-fold improvement compared to conventional photocatalysis while maintaining reaction stability for 120 h. This work provides a novel approach toward green ammonia synthesis and opens new avenues for advancing beyond the fossil fuel driven Haber-Bosch process.
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ORGANOMETALLIC CHEMISTRY
·
2023
·
IF 2.3
Chong Ma,Lei Qin,Zhiping Zheng
Hydrogen, often hailed as the purest form of energy, is renowned worldwide for its exceptional energy density, renewability, and pivotal role in driving sustainable societal progress. However, safe, efficient, and cost-effective storage of hydrogen remains a significant challenge. Ethanol, as a liquid organic hydrogen carrier (LOHC), offers a notable solution with its high hydrogen content, eco-friendliness, and cost efficiency. In this work, hydrogen production by acceptorless dehydrogenation of ethanol (ADE) catalyzed by two new Ru(II) complexes ( C1 and C2 ) with Schiff-base ligands was explored. Under optimized conditions, these catalysts produced respectable turnover numbers (TONs) of 19,398 and 31,965, respectively, comparing favorably with other homogeneous catalysts in the same capacity. Notably, the hydrogen gas produced is free of any CO, which is critical for the hydrogen-based fuel-cell application. Ethyl acetate, the byproduct of this process, can be recycled for other purposes. A mechanism possibly responsible for the observed catalysis was proposed based on an intermediate identified by the mass spectroscopic analysis of the reaction mixture.
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Ming Zhao,Shan Zhang,Yanqing Hu,Huanhuan Xing,Chunmei Li,Weiyong Yuan,Wei Sun,Chunxian Guo,Chang Ming Li
Efficient water splitting electrocatalysts with low cost is essential for the development of sustainable hydrogen energy . Ni foam supported Ru-doped NiCoP nanowire arrays (Ru–NiCoP@NF) are synthesized via a hydrothermal reaction followed by low-temperature phosphorization. The as-obtained Ru–NiCoP@NF exhibits outstanding bifunctional catalytic activity , achieving 100 mA cm −2 at the overpotentials of 108 and 264 mV for HER and OER , respectively, with a tiny loading of Ru (≈61.8 μg cm −2 ). The electrolyzer assembled using Ru–NiCoP@NF as the bifunctional electrode requires 1.62 V (with no iR correction) for 50 mA cm −2 , 50 mV lower than RuO 2 –Pt/C based electrolyzer . The enhancement of Ru–NiCoP@NF is ascribed to Ru dopants , which contribute to formation of 3D nanowire arrays with the advantages of exposing sufficient active sites, accelerating charge transfer and outstanding mechanical strength . More importantly, the Ru atoms in NiCoP successfully modulate the charge densities around Ni, Co and P through strong electronic interaction, thus elevating the sluggish Volmer step for HER and promoting the adsorption capacity of oxygen-containing intermediates for OER .
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Fang Wang,Li-dan Deng,Ze-wei Wu,Kai Ji,Qiao Chen,Xing-mao Jiang
Ru nanoparticles supported on SiO 2 microspheres (Ru/SiO 2 -GUS) were prepared by the glucose-urea-metallic salt method and applied in the decomposition of ammonia. In the glucose-urea-metallic salt method, glucose as the carbon template plays a significant role in the formation of diffusion-beneficial structural properties of Ru/SiO 2 -GUS, and also induceds the modification of the electronic state of Ru. Ru/SiO 2 -GUS exhibited higher catalytic activity compared with the catalyst prepared with the impregnation method. The catalytic performance of Ru/SiO 2 -GUS was further enhanced with the addition of either K or Cs——the addition order and amount strongly affecting the catalytic performance. When the ratio of K/Cs to Ru is 2, the alkali metal (KOH/CsOH) solution is added in the homogeneous solution of glucose, urea, RuCl 3 and the colloidal silica , the promotion effect of K/Cs is the strongest, particularly under lower reaction temperatures. However, the promotion effects of K and Cs are different as reveled by the combined results of H 2 -TPR, XPS and NH 3 -TPSR. More NH 3 can be absorbed on K–Ru/SiO 2 -GUS and the electron density of Ru decreased. By contrast, more metallic Ru formed on Cs–Ru/SiO 2 -GUS, facilitating N 2 recombination.
✓ 已验证
产品关联
DOI
高影响因子