INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2023
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IF 7.2
Yantong Long,Guoliang Zhao,Liuxin Yang,Yuxuan An,Yongjun Xu,Chen Xu
Efficient hydrogen/oxygen evolution reactions (HER/OER) bifunctional catalysts are critical to the overall water splitting efficiency. In this paper, a 1D rod-like structure bifunctional catalyst was firstly prepared, with ultralow Ru (1.19 wt%) loaded into CoNi bimetallic phosphides derived from 1D MOF-74-CoNi nanorods . Due to the strong interface interaction between Co and Ni bimetals which tunes the electronic structure and the Ru loading which increases the number of active sites of the catalyst, the electrocatalytic performance for both HER (8.7mV@10 mA cm −2 ) and OER (179.4mV@10 mA cm −2 ) under alkaline condition were significantly improved. The cell voltage of the full water splitting device assembled by the catalysts was only 1.47 V to achieve 10 mA cm −2 . The rational materials design of 1D rod-like structured bimetallic phosphide catalysts in this work may suggest a new strategy for the preparation of other bifunctional electrocatalysts .
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高影响因子
RENEWABLE ENERGY
·
2021
·
IF 8.001
Feng Lin,Yulong Ma,Yonggang Sun,Kanghe Zhao,Tingting Gao,Yingbo Zhu
Due to the inertness and structural complexity of lignin, upgrading lignin to biofuels and fine chemicals still faces great challenges. In this paper, a one-pot method was used to catalyze straw lignin with H-ZSM-5 supported by Ni and Ru bimetals, and the lignin conversion rate reached 88.1%. The yield of monophenol was 19.5%, of which the yield of 4-ethylphenol and 4-ethylguaiacol was 4.9% and 3.8%, respectively. The 2D HSQC NMR analysis confirmed that the Ni–Ru/H-ZSM-5 catalyst had an obvious activity of breaking C β -O bonds before and after the reaction. The result showed that after loading metal Ni and Ru, the Lewis acid of the catalytic system was greatly increased, which caused electron transfer between Ni and Ru. 3Ni-1.5Ru/H-ZSM-5 had the strongest activity due to the largest synergy among Ni, Ru and H-ZSM-5. The synergy was the key factor leading to the cleavage of C–C and C–O bonds in straw lignin and the high-performance catalytic degradation of lignin. Besides, the effect of reaction solvent and hydrogen resource on upgrading lignin to fine chemicals over 3Ni-1.5Ru/HZSM-5 catalyst was also intensively investigated. This research developed a method for the direct conversion of lignin into valuable monophenols.
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ChemCatChem
·
2020
·Vol. 12
·期 20
·5149-5155
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IF 4.853
Suli Liu,Xueqin Mu,Pengxia Ji,Yun Lv,Lei Wang,Quan Zhou,Changyun Chen,Shichun Mu
Graphical Decorating nanorods : We demonstrate the first metal-phosphides-metal system consisting of Ru and FeCoP, which forms unique CoFeP@Ru nanorod using a simple one-pot synthetic method. Due to its optimal dual cation decorating effects, improved conductivity and rod-like morphology, this catalyst shows superior electro-catalytic HER and OER performances, which are superior to those of some recently reported phosphides and close to that of commercial catalysts. Interfacial engineering and defect modulation can provide abundant active sites for catalysts to further boost the catalysis process. In this work, we develop a strategy to grow multi-heterogeneous cobalt phosphide (CoP) nanorods with rich interfaces and defects along the one-dimensional (1D) nanostructure by dual incorporation of Fe and Ru (CoFeP@Ru). Such a catalyst exhibits high activity and stability towards the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with overpotentials of only 38 mV in 0.5 M H 2 SO 4 and 48 mV in 1.0 M KOH for HER, and an overpotential of 340 mV in 0.1 M KOH for OER at 10 mA cm −2 . Finally, as the bifunctional catalyst, an alkali electrolyzer is assembled and delivers at a low cell voltage, with almost 100 % Faradaic efficiency. Our experimental results demonstrate that Fe incorporation can disturb or even break the periodic structure of cobalt phosphides, causing a redistribution of the electronic structure and electron density of activity sites, while Ru can significantly enhance the catalytic kinetics, as well as electrochemical and mechanical stability.
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ChemNanoMat
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2020
·Vol. 6
·期 8
·1251-1259
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IF 3.384
Wei Cheng,Xue Zhao,Wenxiu Luo,Yun Zhang,Yi Wang,Guangyin Fan
Graphical A bagasse-derived carbon (BC-hs) material with a large surface area (2250 m 2 /g) and abundant surface nitrogen and oxygen species was obtained by a consecutive hydrothermal treatment and solid carbonation. The in-situ formation of Ru/BC-hs with ultrasmall and uniformly dispersed Ru NPs (1.4 nm) provide more catalytically active atoms for AB hydrolysis, achieving a high performance with a TOF of 354 mol H 2 (mol Ru min) −1 . Recently, metal nanoparticles (NPs) have been investigated widely as heterogeneous catalysts in the hydrolysis of ammonia borane (AB). However, the method is severely challenged by the dispersion and particle size of metal NPs, and needs efficient carbon materials as supports. Herein, we describe a facile two-step synthesis strategy that takes advantage of hydrothermal synthesis and solid-phase carbonization to fabricate N-doped bagasse-derived carbon materials (BC-hs). The Ru particles can disperse well on the BC-hs carbon matrix to form Ru/BC-hs catalyst. It is found that the Ru/BC-hs catalyst, under optimized conditions (3.5 wt% Ru loading), shows a high performance for the catalytic dehydrogenation of AB, with a TOF of 354 mol H 2 (mol Ru min) −1 . The high catalytic performance of Ru/BC-hs may be ascribed to the large surface area of BC-hs (2250 m 2 /g) with abundant surface nitrogen and oxygen species, and more catalytically active Ru atoms are provided with the fine-grained and uniformly distributed Ru NPs. This study exhibits a universal method to design and prepare high-performance dehydrogenation catalysts, in which metal NPs are supported on biomass-derived carbon from a highly recyclable and available plant.
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高影响因子
NEW JOURNAL OF CHEMISTRY
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2020
·Vol. 44
·期 27
·11861-11869
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IF 3.288
Shengnan Yue,Xueguang Wang,Shaoting Li,Yao Sheng,Xiujing Zou,Xionggang Lu,Chunlei Zhang
A highly chemoselective and recyclable ruthenium catalyst for the hydrogenation of halogenated nitroarenes has been prepared via the simple in situ calcination of a mixture of melamine, glucose and ruthenium trichloride. Superfine Ru particles (2.3 ± 0.3 nm) were obtained and highly dispersed in the nitrogen-doped carbon matrix. The Ru/CN catalyst smoothly transforms a variety of halogenated nitroarenes to the corresponding haloanilines with high intrinsic activity (e.g. TOF = 1333 h−1 for p-chloronitrobenzene) and selectivity of more than 99.6%. Furthermore, through an analysis of the products in the reaction process, it was concluded that there are two parallel reaction pathways (a direct pathway and an indirect pathway) for the hydrogenation of aromatic nitro compounds over the Ru/CN catalyst, and the direct pathway was proved to be dominant in catalyzing the intermediates.
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CHINESE JOURNAL OF CHEMISTRY
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2020
·Vol. 38
·期 5
·453-457
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IF 3.826
Chuang Li,Guangyue Xu,Xiang Zhang,Yao Fu
Summary of main observation and conclusion The conversion of fructose to 1,2-propylene glycol (PG) is an important process from cellulosic biomass to high-value added chemicals. Herein, Ru-WO x /hydroxyapatite (HAP) catalyst was employed for this reaction and reached up to 91.3% yield of PG at 180 °C, 1 MPa initial hydrogen for 8 h in water. On this catalyst, Ru and WO x were highly dispersed on HAP support and they interacted with each other to form a special catalytic center. The lack of isolated Ru or RuW alloy site led to a moderate activity for hydrogenolysis and hindered the further conversion of PG to propanol. The weak basic HAP support efficiently prevented the humin formation. This precisely controlled catalyst has potential in green PG production.
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高影响因子
CATALYSIS LETTERS
·
2021
·Vol. 152
·期 4
·1170-1181
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IF 3.186
Zhang Xilun,Liu Lin,Feng Ji,Ju Xiaohua,Wang Jiemin,He Teng,Chen Ping
Abstract Development of efficient catalysts for ammonia decomposition is crucial for hydrogen production from ammonia. Herein, Ru nanoparticles (NPs) highly dispersed on Pr 2 O 3 (Ru/Pr 2 O 3 ) were prepared and investigated as catalyst for ammonia decomposition reaction. Under relatively high weight hourly space velocity (WHSV = 30,000 mL g cat −1 h −1 ), the Ru/Pr 2 O 3 achieves a H 2 production rate of 20.9 mmol g cat −1 min −1 at 450 °C, which is superior to Ru/Pr 6 O 11 and many other typical oxides supported Ru catalysts. Detailed characterization results demonstrate that Pr 2 O 3 has high density of basic sites, abundant oxygen vacancies, and strong interaction with Ru, which can modulate electronic properties of Ru NPs and enhance the intrinsic activity of the catalyst, making the catalyst highly active for ammonia decomposition. Moreover, the Ru/Pr 2 O 3 catalyst also exhibits excellent stability and can maintain its high activity for over 100 h. The use of Pr 2 O 3 as support offers opportunity to improve the catalytic performance of Ru-based catalysts for ammonia decomposition. Graphic Abstract
The high density of basic sites, abundant oxygen vacancies of Pr 2 O 3 , and the strong metal–support interaction effectively promote the electron donation to Ru nanoparticles, enabling the superior catalytic performance of Ru/Pr 2 O 3 for ammonia decomposition.
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高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 22
·4814-4823
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IF 5.686
Desen Fu,Xiaoxia Wu,Beilei Cui,Yonghua Guo,Hua Wang,Jinyu Han,Qingfeng Ge,Xinli Zhu
Graphical Solid solution : In contrast to unselective Ru/SiO 2 , solid solution derived Ru 0.05 Ce 0.95 O 2 selectively catalyzes deoxygenation reaction to toluene with significantly inhibited C−C hydrogenolysis and hydrogenation reactions. The Ru−O V −Ce sites are the active sites for deoxygenation, and the inhibition of C−C hydrogenolysis and hydrogenation is due to the reduced Ru ensemble size in the solid solution. Selective hydrodeoxygenation (HDO) of biomass lignin-derived phenolic compounds to aromatics is a demanding reaction. Oxophilic Ru based catalysts can catalyze direct deoxygenation but suffer from competing C−C hydrogenolysis to CH 4 at 350 °C and hydrogenation of phenyl ring at 250 °C under atmospheric pressure. In this work, a solid solution Ru 0.05 Ce 0.95 O 2 catalyst was hydrothermally synthesized, characterized and tested for HDO of m-cresol. The Ru species is highly dispersed in the solid solution as isolated atoms and/or subnanometer clusters as a result of strong Ru−O−Ce interaction, and the catalyst shows high concentration of oxygen vacancies. In contrast to nonselective Ru/SiO 2 , Ru 0.05 Ce 0.95 O 2 selectively catalyzes deoxygenation to toluene while significantly inhibits C−C hydrogenolysis and hydrogenation. Moreover, the overall intrinsic HDO rate on Ru 0.05 Ce 0.95 O 2 is 2.2 and 8.8 times higher than those on Ru/CeO 2 and Ru/SiO 2 , respectively. The Ru−O V −Ce sites were proposed to be the active sites for deoxygenation. Inhibition of C−C hydrogenolysis and phenyl hydrogenation can be ascribed to the reduced size of the Ru ensembles due to the strong interaction in the solid solution.
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JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Xiaohui Yu,Lingyun Dai,Jiguang Deng,Yuxi Liu,Lin Jing,Xing Zhang,Xiyun Jiang,Zhiquan Hou,Jia Wang,Hongxing Dai
SnO 2 is widely used in catalysis owing to its oxygen vacancies, reducible oxygen species, and acidity. In this work, Ru nanoparticles (NPs) supported on three-dimensionally ordered macroporous (3DOM) SnO 2 ( x Ru/3DOM SnO 2 , Ru loading ( x ) = 0.09–1.65 wt%) were fabricated via the polyvinyl alcohol-protected reduction routes, and their catalytic activities were determined for trichloroethylene (TCE) and/or toluene oxidation. It was shown that the 0.98Ru/3DOM SnO 2 sample exhibited the best activity and good thermal stability, with the temperature ( T 90% ) and apparent activation energy at a TCE (1000 ppmv) conversion of 90% being 300 °C and 44 kJ/mol at space velocity = 40,000 mL/(g h), respectively. Trichloromethane, carbon tetrachloride, tetrachloroethylene, and trichloroacetaldehyde hydrate were the main intermediates in TCE oxidation. The high catalytic performance of 0.98Ru/3DOM SnO 2 was attributed to the presence of hydroxyl groups adsorbed at the oxygen vacancies, strong O 2 adsorption ability, good low-temperature reducibility, and strong interaction between Ru NPs and 3DOM SnO 2 . In addition, a catalytic mechanism over x Ru/3DOM SnO 2 was proposed under dry and humid conditions. The introduction of H 2 O could block some of the reaction pathways from inhibiting the production of C 2 Cl 4 , reduce formation of some by-products (e.g., CH 2 Cl 2 , CH 3 COOH, and C 2 H 2 Cl 2 ), promote removal of the chlorine species, and generate a greater amount of HCl and a smaller amount of Cl 2 . Furthermore, introducing toluene into the TCE stream could generate smaller amounts of organic chlorine by-products and greater amounts of inorganic chlorine products (HCl and Cl 2 ). We are sure that this work can provide a guideline for the industrial application of supported Ru catalysts in the removal of Cl-containing volatile organic compounds.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wei Jin,Hengbo Wu,Weiquan Cai,Baohua Jia,Munkhbayar Batmunkh,Zexing Wu,Tianyi Ma
Designing highly-efficient and pH-universal electrocatalysts for overall water-splitting reactions is important for the sustainable production of hydrogen. Herein, NiRu nanoparticles encapsulated into N-doped carbon (NiRu@NC) are fabricated with the assistance of MOF for hydrogen evolution reaction (HER) and also evolved into core–shell structured nanomaterials with abundant interfaces for oxygen evolution reaction (OER, Ni/RuOx@C). Benefiting from optimized electronic structure, interfacial synergy effect and special core–shell structure (~150 nm), the newly developed electrocatalysts present remarkable electrocatalytic activities with small overpotentials to drive 10 mA cm −2 for the HER (19 mV in alkaline, 80 mV in neutral, 20 mV in acid) and OER (252 mV, 316 mV, 211 mV). Moreover, the obtained electrocatalysts exhibit outstanding catalytic performances for overall water-splitting in a two-electrode system with 1.53 V and 1.67 V to drive 10 mA cm −2 in basic and neutral electrolyte, respectively. Remarkably, a small potential of 1.47 V is required to deliver 10 mA cm −2 in acidic media and no significant decay of the activity is observed. This work paves the way for designing a novel class of electrocatalyst that can not only exhibit remarkable electrocatalytic water splitting performances in various conditions, but also possess excellent stabilities for future generation of clean energy.
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Chemistry-An Asian Journal
·
2019
·Vol. 14
·期 16
·2815-2821
·
IF 3.698
Wei Li,Shuang Wang,Jinping Li
Graphical Be well supported ! Two BaCeO 3 supports with strong basic sites were synthesized by a co-precipitation route under different calcination temperatures. BaCeO 3 -a has a high basic density and Ru/BaCeO 3 -a has more oxygen vacancies, which are beneficial for the dissociation of N 2 . Therefore, the 1.25 % Ru/BaCeO 3 -a catalyst exhibits superior performance in ammonia synthesis (see figure). BaCeO 3 -a and BaCeO 3 -b, with strong basic sites, were synthesized by using a co-precipitation method at different calcination temperatures, and used as supports to evaluate their performance in ammonia synthesis. The ammonia synthesis rate with the 1.25 % Ru/BaCeO 3 -a catalyst is 24 mmol g −1 h −1 , which is higher than that of 1.25 % Ru/BaCeO 3 -b catalyst (18 mmol g −1 h −1 ) at 3 MPa and 450 °C. Moreover, the performance of the 4 % Cs-1.25 % Ru/BaCeO 3 -a catalyst was further improved to 28 mmol g −1 h −1 , and no sign of deactivation was observed after a reaction time of 120 h. The XPS and H 2 temperature-programmed reduction analyses indicated that the Ru/BaCeO 3 -a catalyst has more oxygen vacancies than the Ru/BaCeO 3 -b catalyst. In addition, the average Ru particle size of the Ru/BaCeO 3 -a catalyst is closer to 2 nm than the Ru/BaCeO 3 -b catalyst, which promotes the generation of B 5 -type sites (the active site for N 2 dissociation). The CO 2 temperature-programmed desorption analysis indicates that BaCeO 3 -a has a high basic density, which is beneficial for electron transfer to Ru and further facilitates the dissociation of N≡N bonds.
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PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2018
·
IF 3.956
Riyang Shu,Biqin Lin,Jingtao Zhang,Chao Wang,Zhi Yang,Ying Chen
Upgrading of bio-oils to value-added products through simple and cost-efficient catalytic routes is always a big challenge in the energy utilization field. Herein, we prepared a highly dispersed 2 wt% Ru/TiO 2 catalyst using a simple and novel photochemical method at room temperature . The synthetic catalyst exhibited an efficient performance on the HDO of phenolic compounds and real bio-oil, owing to its high Ru dispersion. Guaiacol could be converted into cyclohexane with 91.3% selectivity at 260 °C under 1 MPa H 2 atmosphere. Other typical phenolic monomers (phenol, anisole , etc.) and dimers (α-O-4, 4-O-4, etc.) were transformed into cycloalkanes with most yield close to 100%. Results showed that the cleavage of ether bonds and the HDO step can be realized in one pot. This catalytic system was also effective on the upgrade of bio-oil derived from the pyrolysis of cotton straw. A upgraded product composed of 32.4% hydrocarbons and 57.6% alkylphenols was achieved at 280 °C, which can be used as fuels and chemicals respectively. The enhanced reaction temperature (300 °C) enabled hydrocarbon contents increased to 41.4%, leaving the other oxygenated compounds only 4.2%. This work provides a promising reference for the valorization of raw bio-oil.
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危险品化学品经营许可证（带存储）