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 %.
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Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 38
·13106-13112
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IF 6.4
Mingquan Guo,Jiangnan Shu,Dexin Du,Yisha Wang,Hua Cui
Potential resolved electrochemiluminescence (ECL) nanoluminophores are very important for precise analysis and simultaneous determination of multiple targets. Designing ideal potential resolved ECL nanoluminophores, generating multiple high efficiency ECL emissions without overlap and interference of potential and wavelength, is a challenging subject. Herein, we developed a new nanoluminophore, meso-tetra (4-carboxyphenyl) porphine (TCPP)-functionalized chitosan/Ru(bpy)32+/SiO2 (CRuSiO2) (TCPP@CRuSiO2), with cathode and anode ECL emissions by modifying TCPP on the surface of CRuSiO2 nanoluminophores. The TCPP@CRuSiO2 nanoluminophores presented a uniform sphere morphology (∼50 nm). They exhibited two ECL emissions of 695 nm and 610 nm at −1.20 V and 1.15 V, respectively, by using K2S2O8 and tripropylamine (TPrA) as coreactants. Subsequently, the relevant ECL mechanisms are proposed. In the negative potential range, sulfate radicals (SO4˙−) reacted with TCPP−, generated by the electro-reduction of S2O42− and TCPP, to form the excited state TCPP*, resulting in ECL-1. In the positive potential range, Ru(bpy)33+ and TPrA˙, obtained by electro-oxidation of Ru(bpy)32+ and TPrA, reacted with each other to produce the excited state Ru(bpy)32+*, leading to ECL-2. The synthesized TCPP@CRuSiO2 possesses not only potential and wavelength resolved ECL emissions, but also the advantages of easy synthesis, high ECL efficiency, good stability, and easy film formation on the electrode surface. This work enriches ECL nanoluminophores, which are of important application potential in precise analysis and multiplex analysis.
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ChemNanoMat
·
2023
·Vol. 9
·期 10
·e202300310
·
IF 3.8
Xin Cui,Jiachen Zhang,Yitong Liu,Wen Shao,Yawen Tang,Hanjun Sun
Graphical A Ru-ZIF-8 nanozyme with both esterase like and peroxidase like activities were prepared for acetylcholine (ACh) detection. On the basis of the Ru-ZIF-8 nanozyme, a portable nanozyme strip was developed as a novel biosensor for detecting ACh, which was conducive to promoting the development of multiple enzyme cascade assays. In the present study, the incorporation of Ru into the framework of ZIF-8 resulted in that a Ru-ZIF-8 nanozyme with both esterase-like activity and peroxidase-like activity. Owing to the dual nanozymatic activities of Ru-ZIF-8 nanozyme, the acetylcholine (ACh) detection process utilized only one natural enzyme (choline oxidase), which greatly simplified the detection procedure. In the detection process, nanozyme Ru-ZIF-8 showed esterase-like activity to catalyze the hydrolysis of ACh to choline. Then the generated choline was oxidized by choline oxidase to generate H 2 O 2 . Finally, Ru-ZIF-8 with peroxidase-like activity was used to catalyze H 2 O 2 to oxidize 2,2′-azino-bis (3-ethylbenzothiazo-line-6-sulfonic acid) ammonium salt with a color change. As a result, the linear range for ACh was from 0.01 μM-22 μM with the detection limit (DL) of 5.5 nM. In addition, Ru-ZIF-8 was utilized to fabricate a portable detection test strip. Our work provided a simple, portable, low-cost, highly sensitive and selective assay for the detection of ACh, which paved the way for the development of multi enzyme cascade assays.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yanjun Chen,Yiyang Lee,Wei Chu,Jing Li
The exploitation of highly active and durable electrocatalysts that can replace high-cost Pt/C for hydrogen evolution reaction (HER) is urgently required. The challenge lies in diminishing the usage of noble metals without sacrificing HER activity. In this work, trace Ru-doped transition metal oxides (TMOs) nanoparticles (∼7 nm) with high dispersion loaded by the carbon nanotubes (CNTs) were developed. Specifically, Ru-NiO/CNTs with a low Ru content of 0.94 wt% exhibits excellent alkaline HER activity with the low overpotential of 19 mV and 98 mV to achieve the current density of 10 mA·cm −2 and 100 mA·cm −2 , respectively, outperforming Ru/CNTs counterpart and most previously Ru-based nanocatalysts. Notably, the mass activity (1.83 A·mg Ru -1 ) and price activity (301.51 A·dollar -1 ) of Ru-NiO/CNTs are separately more than 7 times and 18 times higher than that of the commercial 20% Pt/C benchmark. Moreover, the catalyst can operate without activity decay after 100 h long-term stability test. DFT calculation reveals that the synergy effects are originated from (i) the accelerated adsorption and dissociation of H 2 O by Ru, and (ii) the optimized electronic structure of Ni that tunes the H* adsorption/desorption. Furthermore, we discover that Ru-promoted HER activity shows a metal-dependent relationship (Ni ≈ Cu > Mn > Co > Fe), which can use binding energy shift (ΔE) as a highly correlated descriptor. This work may provide an insightful understanding of Ru dopant for enhanced HER activity.
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Catalysis Science & Technology
·
2023
·Vol. 13
·期 14
·4156-4167
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IF 5
Ji Feng,Lin Liu,Xiaohua Ju,Qike Jiang,Jiemin Wang,Jianping Guo,Teng He,Ping Chen
Utilization of promoters to improve the catalytic performance of supported metal catalysts is an important strategy for the design of efficient catalysts. However, it is difficult to detect the relationship between the promoters and the structure of main catalysts. Herein, we firstly develop an efficient Ru-based ammonia synthesis catalyst by decorating Ru nanoparticles (NPs) on γ-alumina with sub-nanometer ceria (CeO2) species (Ce–Ru/Al2O3). In comparison with neat Ru/Al2O3, Ce–Ru/Al2O3 exhibits up to 10-fold activity enhancement at 400 °C and 1.0 MPa. Our characterization results show that such an activity increment is relevant to the function of the sub-nanometer CeO2 species on the Ru NPs. The sub-nanometer CeO2 species will aggregate around the Ru nanoparticles, leading to a clear electron transfer from sub-nanometer CeO2 species to Ru nanoparticles. At the same time, the introduction of CeO2 species can not only weaken the hydrogen poisoning effect on the Ru nanoparticles but also facilitate nitrogen adsorption and hydrogenation of dissociated N* atoms according to the kinetic test results. This work highlights the important role of highly dispersed rare earth oxide promoter species in modulating the structure and catalytic performance of supported Ru NPs for ammonia synthesis.
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APPLIED CATALYSIS A-GENERAL
·
2023
·
IF 5.5
Saisai Wang,Liqi Wan,Chunxiao Jin,Tao Wang,Kaixuan Zhuge,Yuxue Yue,Haiting Cai,Bolin Wang,Renqin Chang,Jia Zhao,Xiaonian Li
Ru-based catalysts have shown great potential for the environmentally friendly industrialization of acetylene hydrochlorination. However, the high cost and reduction of active sites in Ru catalysts have limited their practical applications. In this study, we propose a strategy to optimize the electronic structure of Ru single-atom catalysts by leveraging the strong coordination ability of ligands with the metal and apply this strategy to acetylene hydrochlorination. The experimental results verify that the performance of the catalyst increases with the increase of the ligand. Characterization results indicate that ligands not only optimize the electronic properties of Ru single atoms by forming a RuCl 2 -N structure, but also enhance the adsorption of reactants on the catalysts. DFT calculations reveal that the ligand-modified Ru species can efficiently adsorb and activate acetylene molecules, while the adjacent excessive ligand can adsorb and dissociate HCl molecules. This ultimately leads to an addition reaction between acetylene and HCl through a hydrogen overflow mechanism.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Lidan Deng,Zheng Wang,Xingmao Jiang,Jie Xu,Zijian Zhou,Xiaozhong Li,Zhixiong You,Mingyue Ding,Tetsuya Shishido,Xiaowei Liu,Minghou Xu
Various value-added chemicals such as formic acid , carbon monoxide , methane, methanol, have been obtained using CO 2 as a feedstock. However, formaldehyde generation from CO 2 is less reported. Here, we performed CO 2 hydrogenation with H 2 in additive-free water and used layered double hydroxide supported Ru as the heterogeneous catalyst. It was found that gaseous CO 2 and H 2 could be efficiently and selectively converted to formaldehyde dissolved in water even at room temperature with ambient pressure. The highest gaseous CO 2 conversion of 89.7% and a formaldehyde yield of 58.7% were achieved using a Ru/LDH-red catalyst in water at 30 °C with 10 bar CO 2 and 10 bar H 2 . Combined with experimental and theoretical studies, HCOOH was found as the important reaction intermediate. The rich surface –OH of LDH and hybrid electronic state of Ru over Ru/LDH-red catalyst resulted in highly efficient HCHO formation. Our findings offer opportunities to one energy-efficient formaldehyde synthesis method.
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Chang-An Zhou,Shenghong Wang,Kui Ma,Lei Song,Lirong Zheng,Hairong Yue
The sluggish kinetics and high overpotential of oxygen evolution reaction (OER) at anode hinders water splitting large-scale application. Recently, an anode alternative strategy exhibits promising prospect of application to improve reaction kinetics and decrease overpotential. Here, single dispersed Ru-anchored porous Pt 3 Ni alloy (Ru 1 -Pt 3 Ni/NiF) were successfully synthesized via spontaneous galvanic reduction, over which highly selective electrooxidation of ethanol into acetate was realized. DFT calculations show that Ru modification introduced abundant active oxygen species (OH*), which not only enhanced the oxidation activity of ethanol, but also increased the selectivity for C2 oxidation pathway. Then a Ru 1 -Pt 3 Ni/NiF||Pt 3 Ni/NiF ethanol oxidation membrane-free cell was built to couple the ethanol electrooxidation with H 2 evolution, where the Faraday efficiency of H 2 production reaches 94% and the power consumption is 19.24 kWh kg H2 −1 . This work provides a cost-competitive and energy-saving strategy for high-purity H 2 generation, opening new opportunities for electric energy utilization from renewable sources.
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ChemCatChem
·
2022
·Vol. 14
·期 24
·e202201010
·
IF 5.497
Yanping Hu,Jing Zhou,Xuzhuo Sun,Jing Chen,Bo Li,Yujia Wang,Ning Wang
Graphical Electrocatalytic water-splitting : A facile reduction-hydrolysis strategy was developed to fabricate a Ru−RuO 2 hybrid on various substrates (Ni foam, graphene and CNT) as bifunctional electrocatalysts for water-splitting. Engineering bifunctional nanocomposites with pronounced interfacial structure represents an effective design strategy for water-splitting catalysts. Herein, a facile reduction-hydrolysis method is described for the fabrication of Ru−RuO 2 hybrid nanocomposites on various substrates [Ni foam (NF), carbon nanotubes (CNT) and graphene oxide (GO)] as overall water-splitting catalysts. Polydopamine (PDA) is the key element for simultaneously fabricating the Ru−RuO 2 hybrids as a moderate reductant by controlling the reduction rate. In the synthesis process, a gradual reduction of Ru 3+ to Ru 0 in the presence of PDA occurred during the hydrolytic process of Ru 3+ to form RuO 2 ⋅ n (H 2 O). After calcination, Ru−RuO 2 hybrids with tight interfacial contacts and high electrical conductivity exhibited excellent performance for both HER and OER. Especially, Ru−RuO 2 hybrids on the NF (Ru−RuO 2 /NC/NF) achieved outstanding catalytic activity toward HER and OER with overpotential of 24 mV and 223 mV at a current density 10 mA cm −2 in alkaline solution, respectively. This work provides a new method for facile synthesis and engineering of Ru−RuO 2 nanoparticles on various substrates for boosting the HER/OER performance.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
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.
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Science China-Materials
·
2022
·Vol. 65
·期 10
·2675-2684
·
IF 8.64
Wei Yue,Xu Gao,Wei Yujie,Ji Lvlv,Wang Tao,Liu Zhun,Wang Sheng
Developing highly efficient, cost-effective, and stable electrocatalysts for hydrogen evolution reaction (HER) is of considerable importance but remains challenging. Herein, we report the fabrication of a robust Ru-based electrocatalyst, which comprises heterostructured Ru-Ru 2 P nanoparticles that are embedded in the N,P-codoped carbon nanofibers (CNFs), through a synthetic strategy involving electrospinning and temperature-controlled pyrolysis treatment. The as-prepared Ru-Ru 2 P catalyst (Ru-Ru 2 P@CNFs) shows excellent HER catalytic activities with low overpotentials of 11 and 14 mV in acidic and alkaline media, respectively, to achieve a current density of 10 mA cm −2 , which are superior to the individual components of pure Ru and Ru 2 P catalysts. Density functional theory calculations demonstrate the existence of electronic coupling effect between Ru and Ru 2 P at the heterointerfaces, leading to a well-modulated electronic structure with optimized hydrogen adsorption strength and enhanced electrical conductivity for efficient HER electrocatalysis. In addition, the overall synthetic strategy can be generalized for the synthesis of a series of transitional metal phosphide-based nanofibers, thereby holding a remarkable capacity for various potential applications.
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Green Energy & Environment
·
2022
·
IF 12.781
Yang Yang,Chaoyue Zhao,Xianliang Qiao,Qingxin Guan,Wei Li
In this work, DFT calculations were used firstly to simulate the nitrogen coordinated metal single-atom catalysts (M-N x SACs, M = Hg, Cu, Au, and Ru) to predict their catalytic activities in acetylene hydrochlorination. The DFT results showed that Ru-N x SACs had the best catalytic performance among the four catalysts, and Ru-N x SACs could effectively inhibit the reduction of ruthenium cation. To verify the DFT results, Ru-N x SACs were fabricated by pyrolyzing MOFs in-situ spatially confined metal precursors. The N coordination environment could be controlled by changing the pyrolysis temperature. Catalytic performance tests indicated that low N coordination number (Ru–N 2 , Ru–N 3 ) exhibited excellent catalytic activity and stability compared to RuCl 3 catalyst. DFT calculations further revealed that Ru–N 2 and Ru–N 3 had a tendency to activate HCl at the first step of reaction, whereas Ru–N 4 tended to activate C 2 H 2 . These findings will serve as a reference for the design and control of metal active sites.
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