ACS Sustainable Chemistry & Engineering
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2021
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IF 8.198
Xiaoqing Cao,Jun Zhou,Zhipeng Zhai,Song Li,Guo Yuan,Gaowu Qin
Development of efficient and sustainable monolithic catalysts for NaBH4 hydrolysis remains an important goal for hydrogen cycling. In this work, the structured catalyst Ru/MgO with an on–off feature has been prepared by directly growing a nano-Ru-embedded MgO coating layer on a Mg substrate via an instant high-temperature plasma oxidation process. The porous MgO framework provides an ideal space for the access of reactants and diffusion of mass transport, which facilitates reaction triggering and the expulsion of byproducts to avoid poisoning the catalyst. Importantly, Ru nanoparticles (NPs) are monodisperse with ultrasmall particle size deriving from a concurrent rapid arcing and fast quenching. The hierarchical structured Ru NP catalysts are highly active for hydrolysis of sodium borohydride by achieving a high hydrogen generation rate (HGR) of 101,189 mL min–1 g–1 and exhibit attractive stability. In addition, it is facile to realize the “on–off” functionality based on simple separation that could accurately control the hydrogen generation, suggesting the structured catalyst to be of great potential for practical applications. This simple method opens valuable opportunities for fast synthesis of the high-quality structured catalyst and could be extended to various noble metals on oxides of valve metals with high catalytic performance.
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
高影响因子
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.
研究领域:
催化化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2022
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IF 7.139
Rong Luo,Zhenyu Li,Ruixiang Li,Chunli Jiang,Ruijuan Qi,Mengqin Liu,Hechun Lin,Rong Huang,Chunhua Luo,Hui Peng
It is meaningful to search high-efficient and inexpensive electrocatalysts for hydrogen evolution reaction (HER) due to the energy crisis and environmental pollution. Here, we report the preparation of ultrafine Ru nanoparticles from a hybrid of ZIF-L(Co) MOF and polydopamine coated few-layered Ti 3 C 2 T x MXene (FL-Ti 3 C 2 T x ). FL-Ti 3 C 2 T x is used as a template to grow regular leaf-shaped ZIF-L(Co) nanosheets through the reaction of Co ions anchored on the MXene surface with 2-methylimidazole. The obtained hybrid is then doped with Ru ions through ion exchange between Ru and Co ions, followed by thermal annealing at a temperature of 350 °C in an Ar atmosphere to produce ultrafine Ru nanoparticles. The obtained Ru@ZIF-L(Co)/FL-Ti 3 C 2 T x nanocomposite shows outstanding HER performance with a low overpotential of 16.2 mV at a current density of 10 mA cm −2 , a small Tafel slope of 21.0 mV dec −1 and excellent stability in 1.0 M KOH solution. This work provides a new strategy for the design and synthesis of highly efficient HER catalyst via MOFs with tunable composition and structure.
研究领域:
材料科学
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能源科学
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产品关联
DOI
高影响因子
Research
·
2019
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IF 0
Cai-Juan Liu,Ning-Ning Zhu,Jian-Gong Ma,Peng Cheng
Xylitol is one of the most famous chemicals known to people as the essential ingredient of chewing gum and as the sugar alternative for diabetics. Catalytic hydrogenation of biomass-derived xylose with H2 to produce high-value xylitol has been carried out under harsh reaction conditions. Herein, we exhibit the combination of Ru NPs with an environmentally benign MOF (ZIF-67) to afford a heterogeneous composite catalyst. Complete conversion of xylose with 100% selectivity to xylitol was achieved at 50°C and 1 atm H2. This is the first successful attempt to produce xylitol with ambient pressure H2 as well as the first time to achieve a 100% selectivity of xylitol for applicable catalysts. We also proved the universality of the Ru@ZIF-67 towards other hydrogenation processes. Under 1 atm H2, we achieved 100% conversion and >99% selectivity of 1-phenylethanol at 50°C for the hydrogenation of acetophenone. This is also the first report of hydrogenating acetophenone to 1-phenylethanol under 1 atm H2, which confirms that our result not only contributes to enhance the industrial yields of xylitol and reduces both the economical and energy costs but also provides new perspectives on the other hydrogenation process with H2.
研究领域:
生物化学
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催化化学
✓ 已验证
DOI
CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Huatong Li,Xinran Hu,Lixia Wang,Luyan Shi,Tayirjan Taylor Isimjan,Xiulin Yang
Developing heterostructured catalysts with highly active and reusable is an urgent task to achieve green hydrogen production via NaBH 4 . Herein, we proposed a novel NaCl template method, which involves solid-state physical grinding of metal salts, reducing agents and prepared carbon spheres with the participation of sodium chloride to synthesize Ru-particles decorated CoB 2 O 4 supported on hollow mesoporous carbon nanospheres (Ru/CoB 2 O 4 @C) catalysts for efficient and durable H 2 generation through alkaline hydrolysis of NaBH 4 . The optimized catalyst with a Ru content of 3.0 wt% exhibits a high hydrogen generation rate of 8139 mL min −1 g cat - 1 and a low activation energy of 33.2 kJ mol −1 for NaBH 4 hydrolysis, which is one of the most efficient catalysts reported recently. The extraordinary performance is mainly attributed to the synergistic effect between Ru and CoB 2 O 4 species and abundant oxygen vacancies, which facilitate charge redistribution and provide more active sites, thereby enhancing the catalytic activity. Density functional theory calculations support the proposed Michaelis-Menten mechanism, where BH 4 − and H 2 O are adsorbed on electron-rich Ru and electron-deficient CoB 2 O 4 surfaces, respectively, and the reaction energy barrier for the rupture of the B-H bond as the rate-determining step is only 1.37 eV, synergistically promoting the hydrolysis of NaBH 4 . Our study provides an innovative method for designing efficient and stable catalysts for green hydrogen generation.
研究领域:
材料科学
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催化化学
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能源化学
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产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 12
·期 3
·1005-1016
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IF 6.119
Qiang Zhou,Zijiang Zhao,Zihao Yao,Zhongzhe Wei,Songtao Huang,Fangjun Shao,Aiyuan Li,Jianguo Wang
Modulation of the metal–support interaction plays a key role in many important chemical reactions. Here, by adjusting the reduction method of the catalyst and introducing oxygen vacancies in TiO2 to regulate the interaction between Ru and TiO2, four supported Ru nanocatalysts with different encapsulation degrees and electronic structures were obtained. Ru nanoparticles (NPs) partially encapsulated by TiO2 can achieve the selective hydrogenation of 6-chloroquinoline even at room temperature, with a TOF of 12 h−1. Catalytic characterization and DFT calculations indicated that partially encapsulated Ru NPs not only provided active sites for H2 dissociation, but also reduced the probability of Ru NPs being poisoned. Meanwhile, the oxygen vacancies on the surface of TiO2 can adsorb 6-chloroquinoline molecules and provide additional active sites for hydrogenation via hydrogen spillover. Moreover, the enhanced electron transfer from oxygen-deficient TiO2 to Ru made Ru electron-rich, which repelled C–Cl bonds and effectively prevented the production of dechlorination products.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Xiaoyan Liu,Guojun Lan,Yash Boyjoo,Lihua Qian,Sai Gu,Cameron Alexander Hurd Price,Liang Wang,Ying Li,Jian Liu
Ru/carbon catalyst has been considered as a very active catalyst in aqueous-phase hydrogenation of bio-resourced carbonyl compounds. High dispersion of Ru NPs on a carbon support could enhance catalytic performance. In this work, well dispersed Ru nanoparticles on the surface of carbon spheres have been developed by the introduction of nitrogen-doping. Compared with carbon spheres without N-doping, the incorporation of the N-dopant with in the carbon matrix effectively improved the dispersion of Ru nanoparticles, which was confirmed by X-ray photoelectron spectroscopy (XPS) and CO chemisorption characterizations, finding that the presence of quaternary N was responsible for the high dispersion of Ru nanoparticles. Through adjusting the carbonization temperature from 400 to 850 °C, we have shown that the absolute content of quaternary N can be modulated from 3.2 to 22.4 mg g −1 . As a result, the dispersion of Ru nanoparticles was improved from 29.8% to 70.9%. The Ru/N-CS-850 catalyst revealed excellent catalytic performance (9858 h −1 turnover frequency) for the hydrogenation of levulinic acid to γ-valerolactone, also demonstrated very high catalytic activity for other hydrogenation reactions.
研究领域:
材料科学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
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2023
·Vol. 25
·期 21
·8531-8538
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IF 9.8
Rong Fu,Yan Wang,Guangming Wang,Qingyun Zhan,Lili Zhang,Le Liu
Well-crafted semiconductors exhibiting favorable band structures and strong electron-donating properties can provide a viable pathway for solar-driven nitrogen activation under ambient conditions. In this study, we demonstrate that the nitrogen photo-fixation process can be enhanced by introducing oxygen vacancies and a Ru co-catalyst. The Ru-loaded ZrO2−x photocatalyst achieved an impressive NH3 production rate of 3256 μg g−1 h−1 under visible light irradiation (at 400 nm). Defective ZrO2−x with its enhanced reducing ability and narrow band gap possesses a low work function and excellent electron-donating capability, resulting in remarkable photocatalytic performance for ammonia synthesis under visible light. The supported Ru co-catalyst induces upward band bending in defective ZrO2−x, forming an interfacial Schottky barrier that facilitates the separation of photogenerated charge carriers and provides energetic electrons for nitrogen activation. Mott–Schottky photocatalysts with enhanced back donation ability establish a one-way channel for the transmission of photoexcited electrons, thereby further improving the photocatalytic performance of ammonia synthesis at room temperature.
研究领域:
材料科学
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化学工程
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Yu-Xuan Fu,Shu-Yi Huang,Ming-Shuai Sun,Yan Zhou,Dan-Dan Cai,Wen-Shuai Zhu,Wei Hui,Duan-Jian Tao
Current industrial catalysts for α-pinene hydrogenation suffer from harsh reaction conditions and poor selectivity to cis -pinane, primarily due to their inability to effectively adsorb α-pinene in a specific favorable configuration on the catalyst surface. In this study, a high-specific-surface-area, rod-shaped CeO 2 -supported ultra-fine Ru nanoparticle (average particle size of 4 nm) catalyst was synthesized via hydrothermal method for the highly stereoselective hydrogenation of α-pinene to cis -pinane. The resulting Ru/CeO 2 -H catalyst achieved an α-pinene conversion of 99.3 % and an impressive cis -pinane selectivity of up to 99.6 % under exceptionally low temperature (30°C), 0.6 MPa H 2 and 0.5 h with high TOF (1236 h −1 ). Density functional theory (DFT) calculations indicated that α-pinene preferentially adsorbs onto the Ru surface via the backside of its intramolecular dimethyl bridge. This particular adsorption mode lowers the energy barriers for further hydrogenation to generate cis -pinane. The oriented dimethyl-up configuration of α-pinene and ultra-low activation energy (12.04 kJ/mol obtained from kinetic tests) enable the highly selective production of cis -pinane at ambient temperature. Furthermore, the strong interaction between the CeO 2 -H support and highly dispersed Ru, combined with the ambient-temperature reaction conditions, effectively prevents metal nanoparticle agglomeration and coking, imparting the catalyst with exceptional stability. Notably, the catalyst was reused at least 15 times without observing any significant deactivation, demonstrating its significant potential for practical applications.
研究领域:
催化化学
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材料科学
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理论化学
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产品关联
DOI
高影响因子
Journal of Energy Chemistry
·
2025
·
IF 14.9
Jiayu Xu,Fulin Yang,Xia Guo,Shuli Wang,Ligang Feng
Supported Ru nanoparticles with high utilization are promising for the hydrogen evolution reaction (HER) but the effect of the crystal phase engineering of supports on their performance remains unclear. Here, the impact of the crystal phase of the support on the catalytic activity of Ru was probed by anchoring Ru nanoparticles onto precisely synthesized hexagonal (WO 3 -H), orthorhombic (WO 3 -O), and monoclinic (WO 3 -M) supports followed by thorough evaluation for HER. Among them, WO 3 -H demonstrated superior performance by providing enhanced Ru anchoring and uniform dispersion, maximizing active site availability. A critical finding is the small work function difference (Δ W F ) between Ru and WO 3 -H, which minimizes interfacial charge accumulation and facilitates efficient hydrogen spillover, thereby accelerating HER kinetics. In contrast, WO 3 -O and WO 3 -M exhibited larger Δ W F and less effective Ru dispersion, resulting in a larger hydrogen spillover barrier and suboptimal hydrogen adsorption/desorption dynamics. As a result, Ru/WO 3 -H exhibited the best performance, achieving an overpotential of 43.8 mV at 10 mA cm −2 and a Tafel slope of 49.1 mV dec −1 . This work highlights the critical role of the crystal phase in optimizing the intrinsic catalytic activity of catalysts, offering new insights for designing efficient HER catalysts.
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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2024
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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.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Nanomaterials
·
2015
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IF 1.644
Tong Liu,Qingtao Wang,Bingzheng Yan,Mei Zhao,Wenbo Li,Haiyan Bie
Highly dispersed crystalline Ru nanoparticles (NPs) were successfully immobilized inside the pores of MIL-101 by a double solvents method (DSM). HRTEM clearly demonstrated the uniform distribution of the ultrafine Ru NPs throughout the interior cavities of MIL-101. The synthesized Ru@MIL-101 catalyst was also characterized by X-ray diffraction (XRD), N2 adsorption desorption, and ICP-AES. The catalytic test indicated that the Ru NPs supported MIL-101 material exhibited exceedingly high activity and excellent durability for hydrogen generation from the catalytic hydrolysis of amine boranes.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）