TETRAHEDRON
·
2017
·
IF 2.651
Shi-Yuan Liu,Lin-Yan Xu,Chun-Yu Liu,Zhi-Gang Ren,David James Young,Jian-Ping Lang
An efficient catalytic system containing [RuCl 2 (η 6 -p-cymene)] 2 and one P,N ligand, N-diphenylphosphino-2-aminopyridine ( L1 ) was loaded in catalyzing the alkylation of ketones with primary alcohols for a diverse array of substrates. Other five P,N ligands based on pyridin-2-amine and pyrimidin-2-amine were also examined in this reaction to explore the influence of steric hindrance and electronic effects. Monitoring by 1 H NMR and ESI-MS reveals a stable cationic L1 -coordinated ruthenium hydride intermediate, identified as [Ru(η 6 -p-cymene)(κ 2 - L1 )H] + . Organic intermediates consistent with a three-step dehydrogenation , alkylation and hydrogenation pathway were also observed. The final step in this reaction, the ruthenium-catalysed transfer hydrogenation reduction of α,β-unsaturated ketone with benzyl alcohol was performed separately.
研究领域:
有机化学
·
催化化学
✓ 已验证
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Wei Lv,Xiaohong Hu,Yuting Zhu,Ying Xu,Shijun Liu,Peili Chen,Chenguang Wang,Longlong Ma
Herein, the catalysts of ruthenium and molybdenum oxide nanoparticles supported on activated carbon (AC) were synthesized by precursor stepwise impregnation and employed for the hydrodeoxygenation (HDO) of lignin oil. The XRD, TEM, XPS and NH 3 -TPD-MS result of RuMoO x /AC catalysts confirm that the method of loading molybdenum precursor before ruthenium precursor is advantageous for the MoO x and Ru nanoparticles high dispersion and the reduction of MoO x species enhance the amount of acidity of catalyst. Meanwhile, the reduction temperature of RuMoO x /AC-1-T catalysts could effectively regulate the MoO x species that determine the activity and product distribution of HDO. The conversion of aromatic monomers/dimers were up to 96% with high selectivity of hydrocarbon over RuMoO x /AC-1-350 catalyst at 160 °C and 30 bar H 2 . Which is attributed to the MoO 3 and Ru species possess the excellent activity of benzene ring deep hydrogenation, ether bond breaking and acid dehydration. The RuMoO x /AC-1-350 catalyst effectively converted lignin oil (from the depolymerization of cornstalk hydrolysis residue) into hydrocarbons (56.9 wt%) and cyclohexanol/ethers (18.7 wt%) under 280 °C and 3 bar H 2 . The durability of the RuMoO x /AC-1-350 catalyst for HDO of lignin oil was also investigated and showed that the RuMoO x /AC-1-350 catalyst had good stability, regenerability and repeatability.
研究领域:
催化化学
·
能源化学
✓ 已验证
DOI
高影响因子
Advanced Composites and Hybrid Materials
·
2022
·Vol. 5
·期 2
·696-703
·
IF 11.806
Ge Ruixiang,Chen Liang
RuO 2 has been extensively investigated as a pseudocapacitive material. However, developing a facile and effective method to improve the pseudocapacitive performance of RuO 2 is still desired. In this work, we report the synthesis of ultra-small RuO 2 nanoparticles supported on carbon cloth (us-RuO 2 /CC) via a facile two-step method. As a binder-free electrode, us-RuO 2 /CC exhibits a high capacitance of 1067.4 F g −1 at a current density of 1 A g −1 . Moreover, us-RuO 2 /CC also shows good rate performance (87.8% capacitance retention at 20 A g −1 ) and cycle stability (99.6% capacitance retention after 5000 cycles). Graphical abstract Ultra-small RuO 2 nanoparticles on carbon cloth (us-RuO 2 /CC) were synthesized via annealing and acid etching treatment of a ZnRu precursor, which was prepared by a dip-coating process. Introducing Zn significantly reduces the particle size of RuO 2 , leading to a high specific capacitance of 1067.4 F g −1 .
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2022
·Vol. 14
·期 42
·15724-15734
·
IF 8.307
Shaohua Chai,Shuangde Li,Le Zhang,Guijun Fan,Linfeng Nie,Xin Zhou,Wuxinchen Yang,Weiman Li,Yunfa Chen
The regulation of oxygen vacancies and Ru species using metal–organic frameworks was synergically adopted in a rational design to upgrade Ru/TiO2 catalysts, which are highly active for the catalytic oxidation of dichloromethane (DCM) with less undesired byproducts. In this work, Ru/M-TiO2 and Ru/N-TiO2 catalysts were synthesized by the pyrolysis of MIL-125 and NH2-MIL-125 incorporated with Ru, the existence of Ru nanoclusters and nanoparticles was detected by XAFS, respectively, and the catalytic performance was analyzed comprehensively. Complete oxidation of DCM was obtained at ∼290 °C over Ru/M-TiO2 and Ru/N-TiO2 catalysts, while Ru/N-TiO2 showed quite less monochloromethane (MCM) and higher CO2 yields, and better dechlorination capacity in oxidation. The distinction comes down to that the easier desorption of chlorine could be achieved over Ru4+ which act as the main activated adsorption sites for DCM in Ru/N-TiO2, compared to oxygen vacancies that serve as the main dissociation sites in Ru/M-TiO2. Additionally, Ru/N-TiO2 exhibited superior stability and excellent resilience in moisture. An in situ DRIFTS experiment further indicated the different DCM catalytic degradation process as well as the reaction mechanism over the as-prepared catalysts.
研究领域:
催化化学
·
环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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.
研究领域:
材料科学
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
CARBON
·
2023
·
IF 10.9
Tiantian Ma,Peng Wang,Hua-Jie Niu,Zhongxuan Che,Guozheng Li,Wei Zhou
Exposing more catalytic active sites is an effective strategy to enhance the catalyst activity for hydrogen evolution reaction (HER). Herein, Ti 3 C 2 T x MXene served as a substrate to load thin and curved 2 H –MoSe 2 nanosheets by a typical hydrothermal method , forming MoSe 2 /MXene heterointerface with the fully exposed Mo edge sites. And then, atomically dispersed Ru single atoms (RuSAs) were successfully anchored on the MoSe 2 /MXene (RuSAs@MoSe 2 -MXene). The X-ray absorption near edge structure (XANES) demonstrates that Ru is loaded as single atoms on MoSe 2 and MXene . The prepared sample exhibits improved catalytic activity with a small overpotential of 49 mV at 10 mA cm −2 and a low Tafel slope of 52 mV dec −1 for HER in 0.5 M H 2 SO 4 . It also exhibits excellent stability with a small attenuation voltage of 10 mV for 120 h at 10 mA cm −2 in 0.5 M H 2 SO 4 . When assembled into a two-electrode system of RuSAs@MoSe 2 -MXene||RuO 2 , it only requires a relatively low potential of 1.626 V at 10 mA cm −2 to drive overall water splitting (OWS). Control experiments disclose the highly improved performance can be primarily attributed to the introduced RuSAs and MoSe 2 /MXene heterointerfaces exposing more active sites of Ru and Mo. Moreover, the high conductivity of MXene can increase charge transfer in HER process. The interface engineering with multiple interfaces can provide fresh impetus for the development of efficient HER catalysts.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2019
·Vol. 7
·期 33
·19531-19538
·
IF 10.733
Qi Hu,Guomin Li,Xiaowan Huang,Ziyu Wang,Hengpan Yang,Qianling Zhang,Jianhong Liu,Chuanxin He
Regulation of the electronic structures of metal centers represents a robust strategy for enhancing the activity of electrocatalysts. Herein, we report the crafting of hybrid electrocatalysts comprising both single atomic Ru (SA-Ru) and Ru nanoparticles (NPs) supported on porous N-doped carbon (PC), in which the electronic structures of SA-Ru were effectively optimized by nearby Ru NPs to achieve great enhancement of the hydrogen evolution reaction (HER). The resulting SA-Ru/Ru NPs/PC displayed ultrahigh activity for HER in 1 M KOH with a mass activity of 4.2 mA μgRu−1 at −0.07 V vs. RHE; this activity was 14 times that of commercial Pt/C, representing the largest reported value among the Pt-free electrocatalysts. In addition to the ultrahigh activity, the composite possessed the outstanding stability of 24 h and rapid HER kinetics (i.e. Tafel slope: 31.8 mV dec−1). The experimental and theoretical results matched well with each other and unambiguously indicated that the control over the electronic structures of SA-Ru and the advantageous PC support (i.e. its hierarchical porous nanostructures and superhydrophilic surface) jointly contributed to the exceptional performance.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Zongshan Lin,Shilong Liu,Yonggang Liu,Zhe Liu,Shuidong Zhang,Xiaofeng Zhang,Yong Tian,Zhenghua Tang
Developing efficient, robust, and cost-effective catalysts to boost the electrocatalytic properties of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) for overall water splitting is fundamentally important yet very challenging. Herein, we report a facile method to prepare Ru-based aerogels for HER, OER, and water electrolysis . Specifically, Ru aerogel exhibits comparable HER performance with Pt/C, evidenced by a close overpotential at 10 mA cm −2 , a smaller Tafel slope, and an outperformed long-term stability. Among a series of RuCo aerogels, the Ru 0.7 Co 0.3 aerogel has the best OER performance superior to the RuO 2 benchmark catalyst, with a very small overpotential of 272 mV at 10 mA cm −2 , a low Tafel slope value of 41.6 mV dec −1 , and the improved long-term durability. The excellent OER performance of the Ru 0.7 Co 0.3 aerogel is mainly attributed to the RuCo synergistic catalytic effect, the abundant oxygen vacancies , and the structural merits of the sample. Notably, in the practical overall water splitting test, the combined Ru and Ru 0.7 Co 0.3 aerogel catalyst outperforms the Pt/C + RuO 2 couple. This study can shed light on preparation of metal aerogel-based bifunctional electrocatalyst for overall water splitting and beyond.
研究领域:
材料科学
·
电化学
·
催化
·
能源材料
✓ 已验证
产品关联
DOI
高影响因子
ACS Materials Letters
·
2021
·
IF 8.312
Rui Tang,Zhijie Zhu,Chaoran Li,Mengqi Xiao,Zhiyi Wu,Dake Zhang,Chengcheng Zhang,Yi Xiao,Mingyu Chu,Alexander Genest,Günther Rupprechter,Liang Zhang,Xiaohong Zhang,Le He
Cascade catalysis of reverse water gas shift (RWGS) and well-established CO hydrogenation holds promise for the conversion of greenhouse gas CO2 and renewable H2 into liquid hydrocarbons and methanol under mild conditions. However, it remains a big challenge to develop low-temperature RWGS catalysts with high activity, selectivity, and stability. Here, we report the design of an efficient RWGS catalyst by encapsulating ruthenium clusters with the size of 1 nm inside hollow silica shells. The spatially confined structure prevents the sintering of Ru clusters while the permeable silica layer allows the diffusion of gaseous reactants and products. This catalyst with reduced particle sizes not only inherits the excellent activity of Ru in CO2 hydrogenation reactions but also exhibits nearly 100% CO selectivity and superior stability at 200–500 °C. The ability to selectively produce CO from CO2 at relatively low temperatures paves the way for the production of value-added fuels from CO2 and renewable H2.
研究领域:
化学工程
·
催化
·
能源转换
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2024
·
IF 8.3
Weiwei Han,Xinuo Cai,Jiahong Liao,Yi He,Chunlin Yu,Xingwang Zhang
The development of proton exchange membrane water electrolysis is a promising technology for hydrogen production, which has always been restricted by the slow kinetics of the oxygen evolution reaction (OER). Although IrOx is one of the benchmark acidic OER electrocatalysts, there are still challenges in designing highly active and stable Ir-based electrocatalysts for commercial application. Herein, a Ru-doped IrOx electrocatalyst with abundant twin boundaries (TB-Ru0.3Ir0.7Ox@ITO) is reported, employing indium tin oxide with high conductivity as the support material. Combing the TB-Ru0.3Ir0.7Ox nanoparticles with ITO support could expose more active sites and accelerate the electron transfer. The TB-Ru0.3Ir0.7Ox@ITO exhibits a low overpotential of 203 mV to achieve 10 mA cm–2 and a high mass activity of 854.45 A g–1noble metal at 1.53 V vs RHE toward acidic OER, which exceeds most reported Ir-based OER catalysts. Moreover, improved long-term stability could be obtained, maintaining the reaction for over 110 h at 10 mA cm–2 with negligible deactivation. DFT calculations further reveal the activity enhancement mechanism, demonstrating the synergistic effects of Ru doping and strains on the optimization of the d-band center (εd) position and the adsorption free energy of oxygen intermediates. This work provides ideas to realize the trade-off between high catalytic activity and good stability for acidic OER electrocatalysts.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Nano
·
2025
·
IF 16
Yu Liu,Lu Wu,Yong Wang,Le-Wei Shen,Ge Tian,Lianmeng Cui,Ling Qin,Liang Zhou,Yuexing Zhang,Federico Rosei,Xiao-Yu Yang
Electrolysis of seawater for hydrogen (H2) production to harvest clean energy is an appealing approach. In this context, there is an urgent need for catalysts with high activity and durability. RuO2 electrocatalysts have shown efficient activity in the hydrogen and oxygen evolution reactions (HER and OER), but they still suffer from poor stability. Herein, surface S-doped nanostructured RuO2 (S-RuO2) is rationally fabricated for efficient overall seawater splitting. Doping with S enhances the activity (overpotentials of 25 mV for the HER and 243 mV for the OER), long-term durability (1000 h at 100 mA cm–2), and achieves nearly 100% Faraday efficiency (FE). Moreover, the S-RuO2-based anion exchange membrane seawater electrolyzer requires 2.01 V to reach 1.0 A cm–2 under demanding industrial conditions. Experimental analysis and theoretical calculations indicate that surface S introduction could lower the valence state of Ru, thereby conferring enhanced activity and stability. Furthermore, the nanostructured S-RuO2 electrocatalyst is highly protected by the S-doped surface, which repels Cl– in alkaline seawater. This investigation presents a feasible strategy for designing RuO2-based seawater splitting catalysts with both high performance and good resistance to anodic corrosion.
研究领域:
材料科学
·
电化学
·
能源科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
IF 10.8
Zhisong Liu,Haomiao Xu,Yurui Fan,Wenjun Huang,Feng Yu,Zan Qu,Naiqiang Yan
Ruthenium single-atom catalysts have great potential in ammonia-selective catalytic oxidation (NH3–SCO); however, the stable sp3 hybrid orbital of NH3 molecules makes N(sp3)–H dissociation a challenge for conventional symmetrical metallic oxide catalysts. Herein, we propose a heterogeneous interface reverse atom capture strategy to construct Ru with unique asymmetric Ru1N2O1 coordination. Ru1N2O1/CeO2 exhibits intrinsic low-temperature conversion (T100 at 160 °C) compared to symmetric coordinated Ru-based (280 °C), Ir-based (220 °C), and Pt-based (200 °C) catalysts, and the TOF is 65.4 times that of Ag-based catalysts. The experimental and theoretical studies show that there is a strong d–p orbital interaction between Ru and N atoms, which not only enhances the adsorption of ammonia at the Ru1N2O1 position but also optimizes the electronic configuration of Ru. Furthermore, the affinity of Ru1N2O1/CeO2 to water is significantly weaker than that of conventional catalysts (the binding energy of the Pd3Au1 catalyst is −1.19 eV, but it is −0.39 eV for our material), so it has excellent water resistance. Finally, the N(sp3)–H activation of NH3 requires the assistance of surface reactive oxygen species, but we found that asymmetric Ru1N2O1 can directly activate the N(sp3)–H bond without the involvement of surface reactive oxygen species. This study provides a novel principle for the rational design of the proximal coordination of active sites to achieve its optimal catalytic activity in single-atom catalysis.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）