Catalysis Science & Technology
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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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高影响因子
ACS Sustainable Chemistry & Engineering
·
2026
·Vol. 14
·期 30
·13766-13776
·
IF 7.6
Weng Jiali,Liu Zheng,Wang Hongkun,Chu Dawang
Discarded PVC/cotton waterproof materials pose a significant challenge for sustainable recycling due to the release of corrosive HCl and the formation of sintered carbonaceous residues during conventional thermal processing. Here, we report a synergistic catalytic strategy for the co-conversion of PVC/cotton-based waste into value-added chemicals under mild hydrothermal conditions. Initially, Ru/TiO 2 catalyzes the dehydrochlorination of PVC at 190 ° C; the In Situ-generated HCl serves as a Brønsted acid catalyst to hydrolyze cellulose to glucose, followed by hydrogenation to sorbitol in 61.4% yield. The resulting dehydrochlorinated PVC residue undergoes oxidative aromatization to yield aromatic carboxylic acid, with a liquid product yield of 19.5% and a phthalic acid selectivity of 63.7%. Density functional theory calculations attribute the efficient dechlorination to Ru(1015) sites, which lower the activation energy for HCl elimination by 18.76 kJ mol −1 . This catalytic system demonstrates tolerance toward real-world waste composite materials and establishes a novel pathway for the integrated upcycling of halogenated plastics and lignocellulosic biomass. Life-cycle assessment shows 97% lower global warming potential than incineration, advancing resource circularity and sustainable waste management.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Xiaolong Tan,Xiangguo Zhang,Yushi He,Zeyi Jiang,Cheng Bao,Nien-Chu Lai
Carbon monoxide selective methanation (CO-SMET) holds promise for removing low-concentration CO in the hydrocarbon reforming for hydrogen (H 2 ) production process and is a deep CO removal technology suitable for low-temperature fuel cells. However, developing highly efficient CO-SMET catalysts remains a significant challenge. Herein, we report a supported catalyst (Ru 1.0 (Cl)/TiO 2 ) with highly dispersed ruthenium (Ru) metal on a high-specific-surface-area mesoporous titanium dioxide (TiO 2 ) catalyst. This catalyst exhibits excellent performance in CO-SMET. It can reduce the CO concentration to below 10 ppm in a wide temperature range of 190–300 °C, and the outlet CO concentration can reach an ultra-low level of 0.2 ppm in the optimal temperature zone (210–220 °C). Through XPS and in situ DRIFTS characterizations, the crucial role of Ru–Cl species at the metal-support interface is revealed. The presence of chlorine atoms leads to electron enrichment in the Ru metal, enhancing its adsorption and activation of CO.
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ELECTROCHIMICA ACTA
·
2026
·
IF 5.8
Luping Huang,Xinmeng Xu,Kun Wang,Wantao Zhang,Ziping Liu,Tianyu Qi,Feng Li,Qian Liu,Guiying Xu,Weimin Zhou
Oxygen-vacancy-rich TiO 2-x is uniformly coated on the surface of carbon black substrates. • Ru nanoparticles are highly dispersed on the TiO 2-x support. • TiO 2-x efficiently regulates the electronic structure of Ru sites, thus significantly boosting the electrocatalytic hydrogen evolution performance. The exploration of low cost, highly active, and stable catalysts for the hydrogen evolution reaction (HER) is the key to the future application of electrochemical water splitting. Herein, density functional theory (DFT) calculation results reveal that the oxygen vacancies TiO 2-x can effectively modulate the electron structure of Ru, thereby extremely enhancing the catalytic activity of Ru. Experimentally, to form an integrated nano-heterostructure, a facile approach is designed for the fabrication of super dispersed Ru nano particles on oxygen-deficient TiO 2-x , simultaneously combined with carbon black (CB) as a conductive network. Benefiting from the rich active sites, the optimized Ru/TiO 2-x /CB exhibited excellent catalytic performance, with overpotentials of 56 mV and 112 mV for the HER at a current density of 10 mA cm −2 in 1 M KOH and 0.5 M H 2 SO 4 , respectively. Ru/TiO 2-x /CB demonstrates superior stability and rapid HER kinetics under both acidic and alkaline conditions. Our studies provide a facile and feasible strategy for constructing high-performance water-splitting electrocatalysts. Download: Download high-res image (260KB) Download: Download full-size image
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高影响因子
FUEL
·
2023
·
IF 7.4
Zhuojie Zhong,Bowen Luo,Chengyin Lin,Tao Yin,Zhipeng Tian,Chao Wang,Ying Chen,Yanxue Wu,Riyang Shu
An ultrafast preparation method that coupled the photochemical method with the microfluidic technology to synthesize the highly dispersed Ru/TiO 2 catalyst within only 1 min was proposed. This method had an enhanced electron excitation and a high electron transfer efficiency during the preparation process due to the small dimension of the microchannel, which enabled to shorten the preparation time greatly. Much higher metal reduction efficiency was obtained than that of the single photochemical method, and a high Ru metal dispersion on the TiO 2 surface can be achieved. Moreover, a strong interaction between the metal site and the support was formed, resulting in more spillover hydrogen. This Ru/TiO 2 catalyst presented a high activity on the HDO of phenolic compounds. Guaiacol was converted into cyclohexane with 97.6 % selectivity at 260 °C. The raw lignin-oil also can be upgraded efficiently, with the hydrocarbon content increased from 6.7 % to 69.4 %.
研究领域:
催化化学
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能源化学
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高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Rui Li,Sen Bai,Jianxin Liu,Qing Xi,Long Cao,Jinghao Fan,Yawen Wang,Houfen Li,Huibin Ge,Caimei Fan,Lulu Zhang,Shan Gao,Fangxia Xie,Jiancheng Wang
Photocatalytic water splitting is a promising approach for sustainable green hydrogen production, but its practical deployment is severely hindered by two critical limitations: mandatory H 2 /O 2 separation and the requirement for high-pressure hydrogen storage facilities. To address this long-standing bottleneck, a Ru-TiO 2 /Ti 2 C heterostructured photocatalyst is fabricated via a combined hydrothermal and ball-milling route. Operando spectroscopy and DFT calculations verify a cascade charge and hydrogen transfer pathway: photogenerated electrons migrate from TiO 2 to metallic Ru sites to drive water dissociation into surface H* intermediates, which then spillover onto the Ti 2 C substrate. Owing to the strong atomic hydrogen affinity of Ti 2 C, accumulated H* is immobilized in the Ti 2 C lattice via Ti-H covalent bonds, achieving in-situ atmospheric-pressure hydrogen storage. The optimized composite exhibits an in-situ hydrogen storage capacity of 2.1 wt% at ambient temperature and pressure, with a markedly reduced desorption temperature of 216°C and excellent cycling durability. This work establishes an integrated paradigm of photocatalytic water splitting and low-pressure hydrogen storage, offering a feasible strategy to resolve the inherent H 2 /O 2 separation dilemma and advance the practical application of solar-driven hydrogen production.
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
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2022
·
IF 4.644
Zhun Zhou,Xiaozhong Li,Jinjun Li,Zhixiong You
In the present study, CO 2 methanation with Ru nanoparticles loaded onto three TiO 2 nanocrystal supports (TiO 2 anatase with both exposed (001) facets and oxygen vacancies , TiO 2 anatase with exposed (001) facets and general TiO 2 anatase) was demonstrated. The three samples were denoted as Ar700-R, 700-R and Ana-R, respectively. XRD results confirmed that Ar700-R and 700-R sample exposed (001) facets, XPS and EPR results demonstrated the presence of oxygen vacancies on the surface of Ar700-R. In tests of CO 2 methanation activity, Ar700-R showed the highest CO 2 conversion efficiency of 75% and CH 4 formation rate of 18.84 μmol•g −1 •s −1 (GHSV = was 21600 ml•h −1 •g −1 ) at 400 °C. The enhanced CO 2 methanation activity of Ar700-R was attributed to the co-activity achieved by exposing (001) facets and oxygen vacancies on the surfaces of TiO 2 nanocrystal supports.
研究领域:
化学工程
·
材料科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
研究领域:
催化化学
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生物质能
·
绿色化学
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高影响因子
ACS Applied Materials & Interfaces
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2024
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IF 8.3
Lin Zhang,Xingda An,Kai Feng,Juan Li,Jingjing Liu,Jinxing Chen,Chaoran Li,Xiaohong Zhang,Le He
The interest in introducing light into heterogeneous catalysis is driven not only by the urgent need of replacing fossil energy but also by the promise of controlling product selectivity by light. The product selectivity differences observed in recent studies between light and dark reactions are often attributed to photochemical effects. Here, we report the discovery of a non-photochemical origin of selectivity difference, at essentially the same CO2 conversion rate, between photothermal and thermal CO2 hydrogenation reactions over a Ru/TiO2–x catalyst. While the presence of the photochemical effect from ultraviolet light is confirmed, it merely enhances the catalytic activity. Systematic investigation reveals that the gradual formation of an adsorbate-mediated strong metal–support interaction under catalytic conditions is responsible for the variation in the catalytic selectivity. We demonstrate that differences in product selectivity under light/dark reactions do not necessarily originate from photochemical effects. Our study refines the basis for determining photochemical effects and highlights the importance of excluding non-photochemical effects in mechanistic studies of light-controlled product selectivity.
研究领域:
催化
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化学工程
·
物理化学
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DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2026
·
IF 9.1
Junliang Wang,Linqi Shou,Feiyu Chen,Lifeng Yang,Mengyi Qiu,Senwang Chen,Zhiyan Pan,Zhong-Ting Hu,Mian Hu
Catalytic subcritical water oxidation (CSWO) is a promising technology for treating refractory organic pollutants, yet its application to nitrogen-containing wastewater is limited by inefficient nitrogen conversion and the accumulation of nitrogenous intermediates. Herein, predominantly Ru/TiO 2 single-atom catalysts with tunable oxygen vacancy concentrations were developed for nitrobenzene degradation. The optimized 800-Ru/TiO 2 catalyst achieved mineralization and total nitrogen (TN) removal rates of 87.8% and 85.2%, respectively. A pronounced decoupling between organic matter mineralization and nitrogen conversion was observed, with nitrogen transformation identified as the rate-limiting step. Reaction condition analysis reveals that nitrogen transformation is governed by a competition between selective N 2 formation and over-oxidation to NO 3 − , and the coupling of NH 4 + and NO 2 − is identified as the key pathway for N 2 generation, whereas excessive oxidation promotes nitrate accumulation. The introduction of atomically dispersed Ru significantly enhances nitrogen conversion and shifts the reaction pathway toward selective N 2 formation. Structural characterization and electronic analyses demonstrate that oxygen-vacancy-enriched TiO 2 stabilizes Ru single atoms and induces strong metal-support interaction (SMSI), which is associated with enhances oxidant activation and promotes nitrogen redox coupling. The catalyst exhibits good stability over 92% performance retention after five cycles. This work provides insights into the relationship between catalyst structure, electronic properties, and nitrogen transformation, and offers a strategy for achieving efficient and selective nitrogen removal in CSWO systems.
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ACS Catalysis
·
2025
·
IF 13.1
Kaijie Han,Song Song,Yong You,Xiaoqia Fu,Xingang Li
Ru-based catalysts are widely used for the reductive amination of carbonyl compounds. However, challenges remain, particularly in achieving high catalytic activity under mild conditions. In this study, we report a strategy to simultaneously modulate the electron density of Ru0 and the RuOx/Ru0 ratio by systematically adjusting the calcination temperature. The catalyst calcined at 200 °C demonstrated remarkable performance, achieving a 97.8% yield of furfurylamine at 30 °C, significantly outperforming most previously reported catalysts. Furthermore, it showed compatibility with a range of carbonyl compounds. At 200 °C calcination, the reduced electron density of Ru0 weakened its electron-donating ability, thereby facilitating H2 activation. Meanwhile, this treatment yielded the highest RuOx content and thereby generated the greatest Lewis acid site density, enhancing the adsorption and activation of NH3, furfural, and the Schiff base. Mechanistic studies reveal that the synergistic effect between electron-deficient Ru0 and Lewis acid sites significantly reduced the apparent activation energy for the ammonolysis of Schiff base intermediates, the rate-determining step in reductive amination. This work provides an effective strategy for tuning both the electronic structure of the metal and the acid properties of the catalyst, highlighting the crucial role of metal-acid synergy in promoting Schiff base ammonolysis during reductive amination.
研究领域:
催化化学
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化学反应工程
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材料科学
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有机化学
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物理化学
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高影响因子
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