SOLAR ENERGY
·
2018
·
IF 4.374
Shuo Wang,Bao Liu,Yu Zhu,Zirui Ma,Beibei Liu,Xu Miao,Ruixin Ma,Chengyan Wang
Perovskite solar cells (PSCs) as the most promising alternative to the Si solar cells have been developed rapidly in recent time. Superior electron mobility and conductivity of the compact layer material are necessary for high efficiency in perovskite solar cells by reducing excessive charge accumulation and guaranteeing effective electron injection at the compact layer/perovskite interface. In this study, Ru ions were introduced into traditional compact TiO 2 to improve the electron transporting layer (ETL) properties and conductivity performance. Ru 4+ was discovered in the Ru:TiO 2 according to the result of XPS. The reduced trap-filled limit voltage (V TFL ) of the Ru:TiO 2 compact layers showed that trap density in the Ru:TiO 2 film was lower than that of the pristine TiO 2 film. The PSCs based on 1 mol% Ru:TiO 2 exhibited the suitable band gap, low resistivity and high carrier density, comparing with the undoped compact TiO 2 , the charge transportation at the compact layer/mesoporous layer interface was enhanced with the incorporation of Ru, resulting in the reduction in hysteresis of the device. The power conversion efficiency (PCE) of the Ru-doped compact TiO 2 film based PSCs was improved from 14.83% to 18.35%.
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NEW JOURNAL OF CHEMISTRY
·
2018
·Vol. 42
·期 4
·2476-2482
·
IF 3.201
Fanglin Cai,Wei Su,Hussein A. Younus,Kui Zhou,Cheng Chen,Somboon Chaemchuen,Francis Verpoort
While the role of negatively charged axial ligands (e.g. Cl−, Br− and I−) in tuning the reactivity and stability of molecular Ru water oxidation catalysts was well-documented, less was explored when axial ligands are neutral molecules. In this work, we reported the synthesis and full characterization of [Ru(NCNHCO)(bpy)L]+ complexes (L = DMSO, 1; L = 4-picoline, 2), where L is a neutral axial ligand. The effects of these axial ligands on the stability and reactivity of the catalysts were thoroughly investigated. Both complexes were competent to oxidize water with turnover numbers up to 463 and 107, respectively. Complex 1 initiated the water oxidation involving a PCET process. It was found that complex 2 afforded its corresponding Ru–aqua complex owing to the carboxylate dissociation, while complex 1 exhibited considerable stability in acidic aqueous solutions. On the other hand, in the presence of an oxidant, for complex 1 DMSO/H2O exchange occurred, facilitating water oxidation. In contrast, the Ru–O bond cleavage of complex 2 was inhibited, leading to an inferior catalytic performance.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
IF 14.229
Yuzhi Li,Janel Abbott,Yanchun Sun,Jianmin Sun,Yunchen Du,Xijiang Han,Gang Wu,Ping Xu
Here, in an effort to prepare Ru-based metal organic frameworks, we developed a one-step solvothermal synthesis for Ru nanoassembly catalysts, which consist of ˜4 nm Ru nanoparticles well dispersed on amorphous carbon (Ru/C). The Ru/C catalyst obtained from a mixed solvent of H 2 O and CH 3 CH 2 OH (Ru/C-H 2 O/CH 3 CH 2 OH), featured a chain-like porous structure, provides Pt-like catalytic properties with low overpotentials at −10 mA cm −2 for the hydrogen evolution reaction (HER) within a wide range of pH values, i.e., 35 mV in 0.5 M H 2 SO 4 , 53 mV in 1.0 M KOH, and 93 mV in 3.5 wt% NaCl. Ru/C is also an efficient hydrogen oxidation reaction (HOR) catalyst at all pH values. In the alkaline media, Ru/C-H 2 O/CH 3 CH 2 OH achieves a mass activity of 41.1 mA mg -1 at an overpotential of 50 mV and a high exchange current density (0.65 mA cm −2 ). The work provides a facile strategy to synthesize highly active Ru/C catalysts for bifunctional HER and HOR electrocatalysis.
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ChemCatChem
·
2017
·Vol. 10
·期 6
·1376-1384
·
IF 4.803
Zhaoxia Zheng,Zhicheng Luo,Chen Zhao
Graphical Taking the cross : Morphologically cross-shaped HZSM-5 loaded Ru nanoparticles demonstrate high activity (rate: 7.8 g g −1 h −1 ) in the selective hydrogenolysis of guaiacol to benzene in water with a nearly quantitative yield accompanied with high durability. Hydrogenolysis of C−O bonds is an important tool for synthesis of valuable fuels and chemicals from biomass. In this contribution, we report that morphologically cross-shaped HZSM-5-loaded Ru nanoparticles have demonstrated high activity in the selective hydrogenolysis of guaiacol to benzene in water with 97 % yield and a rate of 7.8 g g −1 h −1 accompanied with high durability. N 2 sorption analysis showed that Ru/HZSM-5 (cross-shaped) had a large mesoporous surface area and pore volume for loading small and uniform Ru nanoparticles, as confirmed by TEM images. The stronger interaction of Ru and cross-shaped HZSM-5 was simultaneously confirmed by a higher hydrogen reduction temperature of RuO 2 on calcined Ru/HZSM-5, a blueshift of Ru δ+ -(CO) n , Ru δ+ -(CO), and Ru 0 -(CO) species in the IR spectra of adsorbed CO, and a higher Ru 3d 5/2 binding energy in X-ray photoelectron spectroscopy measurements. The reaction constant in guaiacol hydrogenolysis to phenol over cross-shaped Ru/HZSM-5 (0.051 min −1 ) was 3–4 times higher than that on spherical and cuboid Ru/HZSM-5 (0.012–0.029 min −1 ) at identical conditions, attributed to the remarkable hydrogenolysis catalytic capability of Ru nanoparticles on cross-shaped HZSM-5. In addition, adsorption of guaiacol and hydrogen was more substantial on cross-shaped Ru/HZSM-5, as evidenced by of IR and mass spectroscopy, respectively. The higher adsorption of guaiacol is attributed to the abundant Lewis acid sites on cross-shaped Ru/HZSM-5, as the Al−OH enriched Lewis acid sites favor the adsorption of oxygen-containing guaiacol. The higher rate constant in the primary step, together with the adsorbed high concentrated reactant and hydrogen (with nearly first-order reaction kinetics) on cross-shaped Ru/HZSM-5, facilitates the overall tandem reaction, leading to an excellent hydrogenolysis catalyst working at hydrothermal conditions for biomass conversion.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 30
·2401694
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IF 27.4
Yin Zhu,Yanxu Chen,Yafei Feng,Xiangmin Meng,Jing Xia,Genqiang Zhang
Hydrazine oxidation-assisted water splitting is a critical technology to tackle the high energy consumption in large-scale H 2 production. Ru-based electrocatalysts hold promise for synergetic hydrogen reduction (HER) and hydrazine oxidation (HzOR) catalysis but are hindered by excessive superficial adsorption of reactant intermediate. Herein, this work designs Ru cluster anchoring on NiFe-LDH (denoted as Ru c /NiFe-LDH), which effectively enhances the intermediate adsorption capacity of Ru by constructing Ru─O─Ni/Fe bridges. Notably, it achieves an industrial current density of 1 A cm −2 at an unprecedentedly low voltage of 0.43 V, saving 3.94 kWh m −3 H2 in energy, and exhibits remarkable stability over 120 h at a high current density of 5 A cm −2 . Advanced characterizations and theoretical calculation reveal that the presence of Ru─O─Ni/Fe bridges widens the d-band width (W d ) of the Ru cluster, leading to a lower d-band center and higher electron occupation on antibonding orbitals, thereby facilitating moderate adsorption energy and enhanced catalytic activity of Ru.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2016
·
IF 3.205
Zhiming Gao,Lin Cui,Hongwei Ma
Four methods were adopted to prepare samples 20%NiO/Al 2 O 3 with calcination fixed at 500 °C, which were then reduced into 20%Ni/Al 2 O 3 and used as catalysts for reaction of selective methanation of CO in H 2 -rich gas (CO-SMET). XRD and TPR measurements indicate that nickel aluminates were formed in the calcined samples and their formation was influenced by preparation methods. Higher temperatures were required to reduce the calcined samples more efficiently and to achieve a higher catalytic activity for CO-SMET. Among the four methods, the precipitation method using ammonium carbonate as precipitant produced the highest catalytic activity both for CO methanation and for CO 2 methanation after reduction at 800 °C for 2 h. The calcined sample 20%NiO/Al 2 O 3 prepared with the method was therefore used as support and impregnated with Ru 3+ solution. Ru addition promoted reduction of Ni 2+ ions in the calcined sample even at the low temperatures of 400 °C and 500 °C. The catalyst 1%Ru–20%Ni/Al 2 O 3 reduced at 500 °C thus had a superior performance, removing CO to ca. 30 ppm with a selectivity as high as 75% at reaction temperature of 220 °C.
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ACS Catalysis
·
2015
·
IF 9.312
Liang Wang,Jian Zhang,Xianfeng Yi,Anmin Zheng,Feng Deng,Chunyu Chen,Yanyan Ji,Fujian Liu,Xiangju Meng,Feng-Shou Xiao
Zeolite-based catalysts have been widely used in the conversion of biomass recently, but the catalytic yields of the desired products are strongly limited by the relatively small micropores of zeolite. Here, we reported a hierarchically porous ZSM-5 zeolite with micropore and b-axis-aligned mesopore-supported Ru nanoparticles (Ru/HZSM-5-OM) that are highly efficient for the hydrodeoxygenation of both small and bulky phenolic biomolecules to the corresponding alkanes. Compared with the conventional ZSM-5 zeolite-supported Ru catalyst, the high catalytic activities and alkane selectivities over Ru/HZSM-5-OM are attributed to the abundant exposed acidic sites in HZSM-5-OM with open mesopores. This feature is potentially important for future phenolic bio-oil upgrading.
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Small
·
2024
·
IF 13
Yingyan Ma,Yuan Ha,Liangqiang Chen,Ziqi An,Linzhuang Xing,Zhenni Wang,Zhimin Li
Efficient and affordable price bifunctional electrocatalysts based on transition metal oxides for oxygen and hydrogen evolution reactions have a balanced efficiency, but it remains a significant challenge to control their activity and durability. Herein, a trace Ru (0.74 wt.%) decorated ultrathin CoOOH nanosheets (≈4 nm) supported on the surface of nickel foam (Ru/CoOOH@NF) is rationally designed via an electrochemically induced strategy to effectively drive the electrolysis of alkaline overall water splitting. The as-synthesized Ru/CoOOH@NF electrocatalysts integrate the advantages of a large number of different HER (Ru nanoclusters) and OER (CoOOH nanosheets) active sites as well as strong in-suit structure stability, thereby exhibiting exceptional catalytic activity. In particular, the ultra-low overpotential of the HER (36 mV) and the OER (264 mV) are implemented to achieve 10 mA cm −2 . Experimental and theoretical calculations also reveal that Ru/CoOOH@NF possesses high intrinsic conductivity, which facilitates electron release from H 2 O and H-OH bond breakage and accelerates electron/mass transfer by regulating the charge distribution. This work provides a new avenue for the rational design of low-cost and high-activity bifunctional electrocatalysts for large-scale water-splitting technology and expects to help contribute to the creation of various hybrid electrocatalysts.
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JOURNAL OF THE ENERGY INSTITUTE
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2024
·
IF 5.6
Bo Chen,Qing-Pan Du,Zhi-Jun Diao,Hong Yuan,Jia-Meng He,Yi-Qing Xie,Xiao-Ran Wang,Yu Wang
Hydrogenation upgrading is an effective technique that lowers the oxygen content of bio-oil with the aim of improving its quality. In order to fabricate a series of Ru-based catalysts for the hydrodeoxygenation of bio-oil, several all-silica supports with different pore sizes are synthesized and modified with Al and Cs in this work. The physical morphology and electronic structure of the catalysts are characterized using multiple techniques including X-ray diffraction, in-situ pyridine adsorption infrared spectroscopy, in-situ diffuse reflectance Fourier transform infrared spectroscopy , Raman spectroscopy , CO 2 temperature-programmed desorption, scanning electron microscopy, energy-dispersive X-ray spectroscopy, transmission electron microscopy , X-ray photoelectron spectroscopy and N 2 physical adsorption-desorption testing. Phenol , guaiacol , anisole and o-cresol are selected as model compounds to investigate the hydrodeoxygenation reactivity of the catalysts. The results reveal that there is a strong linear correlation between the pore size of the catalysts and the rates of the hydrogenation and hydrodeoxygenation of phenol. Importantly, both the oxygen vacancy density and relative content of Brønsted and Lewis sites (B/L) of the catalysts can be greatly increased by Cs modification, which further linearly promotes the hydrodeoxygenation activity of the catalysts. In addition, the in-situ infrared spectroscopy results show that the catalysts modified by Al and Cs heterolytically cleave H 2 to supply H + for the reaction. This work presents a novel approach for fabricating catalysts employed in the hydrotreatment process of bio-oil.
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Nature Communications
·
2024
·Vol. 15
·期 1
·1-10
·
IF 14.7
Tang Minhao,Shen Ji,Wang Yiding,Zhao Yanfei,Gan Tao,Zheng Xusheng,Wang Dingsheng,Han Buxing,Liu Zhimin
The chemical recycling of polyester wastes is of great significance for sustainable development, which also provides an opportunity to access various oxygen-containing chemicals, but generally suffers from low efficiency or separation difficulty. Herein, we report anatase TiO 2 supported Ru and Mo dual-atom catalysts, which achieve transformation of various polyesters into corresponding diols in 100% selectivity via hydrolysis and subsequent hydrogenation in water under mild conditions (e.g., 160 °C, 4 MPa). Compelling evidence is provided for the coexistence of Ru single-atom and O-bridged Ru and Mo dual-atom sites within this kind of catalysts. It is verified that the Ru single-atom sites activate H 2 for hydrogenation of carboxylic acid derived from polyester hydrolysis, and the O-bridged Ru and Mo dual-atom sites suppress hydrodeoxygenation of the resultant alcohols due to a high reaction energy barrier. Notably, this kind of dual-atom catalysts can be regenerated with high activity and stability. This work presents an effective way to reconstruct polyester wastes into valuable diols, which may have promising application potential.
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NEW JOURNAL OF CHEMISTRY
·
2024
·Vol. 48
·期 24
·11079-11089
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IF 2.7
Xi Hu,Yujun Yang,Yaoyang Pu,Weiwei Zhang,Xiang Mao
The ruthenium (Ru)-based functional structure has been well understood in catalytic performance due to its special particularity in structural fabrication. In this work, the controllable synthesis of core–shell Ru nanomaterials is first reported, which were not only realized via ice bath conditions with amorphous characterization but also showed a flexible design in the controllable synthesis of crystalline Ru after high intensity focused ultrasound (HIFU) treatment. The achieved amorphous Ru particles (∼115 ± 3 nm) and crystalline Ru (∼5 ± 0.5 nm) exhibit hydrogen peroxide catalytic performance and can be considered as an electrochemical sensing platform. The Km value of core–shell Ru for 3,3′,5,5′-tetramethylbenzidine (TMB) was 0.221 mM, which exhibits higher affinity for TMB and prominent catalytic performance than horseradish peroxidase (HRP). For selectivity and sensitivity towards the detection of H2O2 molecules, it expressed a wide linear range from 0.5 to 100 mM with an H2O2 detection limit of 1.45 μM (S/N = 3) and a sensitivity of 2.07 μA μM−1. After HIFU treatment, the diameter of the achieved crystalline Ru was about one-twentieth that of the core–shell Ru structure. An enhancement in catalytic performance was observed as a sensor platform for detecting H2O2, its detection range was wider, from 0.5 to 110 mM, its limit of detection was 0.007 μM (S/N = 3), and it exhibited a higher sensitivity of 443 μA μM−1. Hence, this flexible design in the synthesis of Ru NMs (amorphous and crystalline in status) could provide a novel synthetic strategy and make achievements in catalytic performance.
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Science Bulletin
·
2025
·
IF 21.1
Qingyu Wang,Yangyang Wan,Qichen Liu,Yida Zhang,Zhentao Ma,Zirui Xu,Pengting Sun,Gongming Wang,Hai-Long Jiang,Wenping Sun,Xusheng Zheng
Photocatalytic urea production from nitrogen (N 2 ) and carbon dioxide (CO 2 ) is a sustainable and eco-friendly alternative to the Bosch-Meiser route. However, it remains a significant challenge in developing highly efficient photocatalysts for enhancing C-N coupling to high-yield urea synthesis. Herein, we propose a multi-site photocatalyst concept to address the concern of low yield by simultaneously improving photogenerated carrier separation and reactant activation. As a proof of concept, a well-defined multi-site photocatalyst, Ru nanoparticles and Cu single atoms decorated CeO 2 nanorods (Ru-Cu/CeO 2 ), is developed for efficient urea production. The incorporation of Ru and Cu sites is crucial not only to generate high-density photogenerated electrons, but also to facilitate N 2 and CO 2 adsorption and conversion. The in situ formed local nitrogen-rich area at Ru sites increases the encounter possibility with the carbon-containing species generated from Cu sites, substantially promoting C-N coupling. The Ru-Cu/CeO 2 photocatalyst exhibits an impressive urea yield rate of 16.7 μmol g −1 h −1 , which ranks among the best performance reported to date. This work emphasizes the importance of multi-site catalyst design concept in guaranteeing rapid C-N coupling in photocatalytic urea synthesis and beyond.
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