JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Da Yang,Cong-Kun Zhong,Lu-Yao Tian,Long-Li Zhang,Huan Liu
Formic acid (FA) is a potential hydrogen storage substance due to its abundant resources, ease of storage, and high hydrogen content. In this paper, the hydroaminomethylation of olefins with FA as the hydrogen source was accomplished over DPEPhos-based Ru catalyst for the first time. Under optimal conditions, α-olefins or cycloolefins with steric hindrance obtained 62%∼96% yields of the target amines. The influence of FA was investigated by in situ high-pressure 1 H NMR spectroscopy analyses, isotope labelling experiments, and the separated hydroformylation or reduction amination. It was indicated that FA was decomposed to provide H 2 for the hydroformylation, and was used as a reducing agent in the transfer hydrogenation of imines/enamines. The reversible amidation of FA with substrate amine could inhibit the side reaction of aldehydes transfer hydrogenation. Moreover, the involving FA would facilitate the formation of Ru-H species, thereby promoting the hydroaminomethylation.
研究领域:
化学
·
催化科学
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DOI
高影响因子
Journal of the American Chemical Society
·
2018
·
IF 14.357
Jinghua An,Yehong Wang,Jianmin Lu,Jian Zhang,Zhixin Zhang,Shutao Xu,Xiaoyan Liu,Tao Zhang,Martin Gocyla,Marc Heggen,Rafal E. Dunin-Borkowski,Paolo Fornasiero,Feng Wang
The interface of metal-oxide plays pivotal roles in catalytic reactions, but its catalytic function is still not clear. In this study, we report the high activity of nanostructured Ru/ceria (Ru-clusters/ceria) in the ethylene methoxycarbonylation (EMC) reaction in the absence of acid promoter. The catalyst offers 92% yield of MP with TOF of 8666 h–1, which is about 2.5 times of homogeneous Pd catalyst (∼3500 h–1). The interfacial Lewis acid–base pair [Ru-O-Ce-Vö], which consists of acidic Ce-Vö (oxygen vacancy) site and basic interfacial oxygen of Ru-O-Ce linkage, acts as active site for the dissociation of methanol and the subsequent transfer of hydrogen to the activated ethylene, which is the key step in acid-promoter-free EMC reaction. The combination of 1H MAS NMR, pyridine-IR and DFT calculations reveals the hydrogen species derived from methanol contains Brönsted acidity. The EMC reaction mechanism under acid-promoter-free condition over Ru-clusters/ceria catalyst is discussed.
研究领域:
催化化学
·
材料科学
·
表面科学
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DOI
PubMed
高影响因子
FUEL
·
2025
·
IF 7.5
Qijing Zhang,Hongxia Yu,Siyi Wang,Haibo Li,Suyuan Zeng,Rui Li,Qingxia Yao,Qi Zhang,Ruru Chen,Lijian Meng,Konggang Qu
Overall water splitting (OWS) is the most potential method for large-scale hydrogen production, but the high-potential and sluggish oxygen evolution reaction (OER) greatly impedes its efficacy. Coupling the low-potential hydrazine oxidation reaction (HzOR) with the cathodic hydrogen evolution reaction (HER) has drawn widespread attention with energy-saving advantage and safe products, which necessitates the elaborate design of advanced bifunctional electrocatalysts. Herein, only using two complexes of Ru and Pd with 2,2′-bipyridine, the novel RuPd alloy/N-codoped carbon (RuPd/NC) composite was originally synthesize by direct mixing and pyrolysis, showing superior dual activity for HER and HzOR. Particularly, to deliver the current density of 10 mA cm −2 , RuPd/NC merely needs the potentials of −8 and −42 mV for alkaline HER and HzOR, far outperforming Pt/C and being most advanced among the previously studied counterparts. Moreover, the two-electrode overall hydrazine splitting (OHzS) needs ultrasmall voltages of 0.042 and 0.239 V to achieve 10 and 100 mA cm −2 , displaying great energy-saving feature. Moreover, the better activity for neutral HER, HzOR and OHzS on RuPd/NC was also found compared with Pt/C. The theoretical simulations uncover the water dissociation at Ru site with the greatly reduced energy barrier followed by the H desorption on the adjacent Pd site for HER, and the optimum activation energy on Ru site for HzOR, crediting to the synergistic regulation of alloying effect and metal-substrate interaction.
研究领域:
电催化
·
材料化学
·
能源科学
·
纳米材料
·
物理化学
·
可持续能源技术
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DOI
高影响因子
BIOMASS & BIOENERGY
·
2025
·
IF 5.8
Shiting Chen,Sisi Jia,Nan Xi,Qinglian Wang,Yixiong Lin,Chen Yang,Wang Yin,Ting Qiu
Noble metal catalysts, particularly Ru-based, demonstrate exceptional activity during catalytic hydrotreatment of fast pyrolysis liquids (PLs) from lignocellulosic biomass. However, their high cost poses a major barrier to practical applications. Herein, a series of cost-effective bimetallic Ru-Ni catalysts with varying Ru/Ni ratios (5 wt% metal loading, Ru x Ni y /NC) supported on hierarchical nitrogen-doped carbon materials (NC) were facilely prepared by the wet impregnation method. The performance was evaluated for catalytic hydrotreatment of PLs. The results revealed that the introduction of Ni to Ru significantly enhances catalytic performance. Among the tested catalysts, Ru 4 Ni 1 /NC exhibited optimal activity, achieving the product oils with the highest H/C ratio and lowest thermogravimetric (TG) residue. Under mild condition (200 °C, 6 MPa H 2 , 4 h), the catalyst yielded the product oil with an H/C ratio of 1.49 and a TG residue of 10.7 wt%. When subjected to deep hydrotreatment condition (340 °C, 6 MPa H 2 , 4 h), the catalyst generated the product oil with an H/C ratio of 1.32 and a TG residue of 2.9 wt%. To gain insights into the catalytic mechanism, the adsorption behavior of model components in PLs onto the catalyst was investigated through FT-IR. The results revealed that the incorporation of low electronegativity Ni to Ru, induces the electron transfer from Ni to Ru, resulting in electron enrichment at Ru sites and electron deficient at Ni sites, which promotes the adsorption of substrates onto the catalyst, thereby boosting hydrogenation of PLs. These findings highlight the significant potential of bimetallic Ru-Ni/NC for catalytic hydrotreatment of PLs into intermediates that can be co-processed with vacuum gas oil in FCC refinery for biofuel production.
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高影响因子
NEW JOURNAL OF CHEMISTRY
·
2020
·Vol. 44
·期 19
·7962-7967
·
IF 3.288
Zichuang Li,Yu Pei,Qiangjian Ju,Beibei Guo,Yifan Hu,Qian Liu,Yufang Zhu,Jiacheng Wang
The preparation of a highly active, cost-effective catalyst is the key to the commercial production of hydrogen through the electrochemical splitting of water, which is an ideal route to a clean energy conversion and storage system in the future. Unfortunately, the current catalysts for HER are rarely able to balance performance and cost. Herein, we successfully prepared an efficient catalyst (Ru/N–C) for HER by a facile method through a multi-step pyrolysis hard template. The electrochemical tests show that the HER activity of the synthesized Ru/N–C-6% catalyst with an onset potential of 0 mV and an overpotential of 34 mV at 10 mA cm−2 was comparable to that of Pt/C in 1 M KOH. Moreover, after 10 000 cycles, the potential change at 10 mA cm−2 is almost negligible. The origin of this high activity was analyzed via density functional theory (DFT), and the mechanism is further understood. Therefore, this work provides a promising substitute for Pt-based catalysts.
研究领域:
材料科学
·
能源化学
·
理论计算
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2018
·
IF 6.14
Xia Cheng,Hua Wang,Mei Ming,Wenxiu Luo,Yi Wang,Yingchun Yang,Yun Zhang,Daojiang Gao,Jian Bi,Guangyin Fan
Developing efficient and affordable alternatives for Pt-based electrocatalysts to promote the procedure of hydrogen evolution reaction (HER) is of significant importance. Herein, a facile and convenient strategy using tris(2,2′-bipyridyl)ruthenium(II) chloride hexahydrate as precursor is developed for synthesizing ultrafine and highly dispersed ruthenium nanoclusters on carbon support. It is discovered that the preadsorption of Ru precursor on carbon substrate and followed by pyrolysis are very crucial for the synthesis of such Ru nanoclusters. Among as-prepared samples, Ru/CN-800 shows the best HER electrocatalytic performance in alkaline solution, which outperforms the benchmark Pt/C and recently reported catalysts. The excellent performance of Ru/CN-800 was presumably attributed to the dominant metallic Ru as well as the ultrasmall Ru nanoclusters with a satisfied dispersion, which provides the massive highly active sites for HER. This facile and environmental-friendly pathway for synthesis of ultrasmall Ru nanoclusters with high HER activity shows a promise in practical applications.
研究领域:
材料科学
·
电化学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Zengfu Zhang,Haiqing Wang,Mingjun Ma,Huiling Liu,Zhicheng Zhang,Weijia Zhou,Hong Liu
Cooperative promotions of intrinsic activity, active sites amount, and mass transfer/charge transport in electrocatalytic process are highly depending on the fundamental understanding of reaction mechanism and the systematic and elaborate designing of morphological, electronic, and interfacial structure of electrocatalyst. Herein, a hybrid nanostructure of RuO 2 strongly coupled with structurally controllable NiMoO wafer arrays was elaborately fabricated via highly matched lattices for superior alkaline water electrolysis through optimizing the adsorption energies of the key intermediates at the interface based on synergistic electronic, geometric, and interfacial effects. The incorporation of Mo ion can adjust the electronic structure of host NiO x endowing the resultant NiMoO with suitable H and O intermediate binding energy for active species transfer between the interfaces. The ratio of O/C on the surface of flexible carbon cloth was well tuned through O 2 -plasma to achieve the desired geometric structure of NiMoO wafers with features of rich porosity and abundant active site. The RuO 2 nanoparticles are homogeneously distributed on the surface of porous NiMoO wafers via highly matched lattices, thereby offering efficient interfacial synergy. Consequently, the hybrid nanostructure of Ru species and NiMoO exhibits greatly enhanced bifunctional electrocatalytic activities toward both HER and OER for overall water splitting. The integrated NiMoO wafer works like a turbo for engineering robust Ru-based bifunctional electrocatalyst. The finding may provide insights for the rational design of advanced nanocomposite catalysts for various energy conversion applications.
研究领域:
材料科学
·
电化学
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DOI
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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高影响因子
Journal of Energy Chemistry
·
2026
·
IF 15.6
Xiaoxiao Duan,Suya Li,Xiuling Jiao,Yuguo Xia,Dairong Chen
Ruthenium oxide is among the most active electrocatalysts for the acidic oxygen evolution reaction (OER), yet its practical use is severely limited by anodic over-oxidation, lattice-oxygen participation, and the resulting Ru dissolution. Here, we report a monolithic RuO 2 -TiO x /Ti anode directly constructed on Ti felt through a one-step impregnation-calcination strategy, in which the native surface oxide evolves at only 400 °C into a rutile-like TiO x interlayer that is lattice-matched with rutile RuO 2 . The resulting structurally defined RuO 2 -TiO x heterointerface induces interfacial charge redistribution and tensile lattice distortion, thereby modulating the Ru–O coordination environment, attenuating Ru–O covalency, and suppressing excessive lattice-oxygen participation. Operando spectroscopy, isotope-labeling analysis, electrochemical probing, and theoretical calculations collectively reveal that such interfacial regulation shifts acidic OER toward the adsorbate-evolution mechanism while suppressing Ru overoxidation and local structural reconstruction. Beyond active-site modulation, the integrated TiO x interlayer and metallic Ti scaffold provide robust interfacial adhesion, efficient electron transport, and favorable gas/liquid transport under high-rate operation. As a result, RuO 2 -TiO x /Ti delivers an overpotential of 172 mV at 10 mA cm −2 , sustains 50 mA cm −2 for 1000 h with only 18 ppb Ru dissolution, and enables proton exchange membrane (PEM) water electrolysis at 1.65 V at 1 A cm −2 . This work highlights lattice-matched heterointerface engineering as an effective strategy for durable acidic OER electrodes. The lattice-matched RuO 2 -TiO x heterointerface induces charge redistribution and tensile distortion, elongating Ru–O bonds, reducing covalency, and suppressing lattice-oxygen participation for highly active and durable acidic oxygen evolution reaction (OER). Download: Download high-res image (145KB) Download: Download full-size image
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高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2026
·
IF 19.9
Shuyu Jia,Xin Zhang,Yuejia Guo,Jiachen Zhang,Qicheng Liu,Shen Wang,Yawen Tang,Jiali Wang,Yu Wang,Hanjun Sun
Phase engineering effectively modulates the strong metal-support interaction (MSI) in heterogeneous catalysts. However, the dynamic manipulation of MSI through in situ phase transition remains underexplored. Herein, an acid-mediated strategy for in situ 1T→2H phase transformed MoSe 2 has been reported to construct Ru sites (Ru-2H(PT)-MoSe 2 /CC) toward alkaline hydrogen evolution reaction, in contrast to direct Ru sites construction on the static 2H-phase MoSe 2 (Ru-2H-MoSe 2 /CC). X-ray photoelectron spectroscopy demonstrates that, despite both catalysts sharing the same 2H-phase structure, the phase-evolved Ru-2H(PT)-MoSe 2 /CC exhibits significant electron accumulation at Mo and Se sites, enabling strong electrostatic interaction with the Ru 3+ precursor, which dictates the final atomic configuration of Ru. Combined theoretical and experimental studies demonstrate that this strong MSI preferentially stabilizes Ru as single atoms at Mo sites concurrently with the formation of smaller Ru clusters. In stark contrast, the weak MSI in Ru-2H-MoSe 2 /CC leads to the predominant formation of larger Ru clusters. The resultant Ru-2H(PT)-MoSe 2 /CC yields a low overpotential of 26 mV at 10 mA cm −2 and long-term durability for 500 h at 100 mA cm −2 . In situ Raman spectroscopy and theoretical calculations further corroborate that the unique Ru configuration optimizes interfacial water behavior and accelerates water dissociation kinetics.
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高影响因子
Catalysts
·
2026
·Vol. 16
·期 2
·185
·
IF 4.5
Jie Yang,Yongsheng Liu,Xiaowen Guo,Qi Yang,Yejun Guan
Gamma-valerolactone (GVL) can be used as a renewable solvent, flavoring agent, and precursor to produce liquid fuels and fine chemicals. GVL is mainly produced by the efficient hydrogenation of levulinic acid and its esters over a wide range of bifunctional catalysts under harsh conditions because high temperature is generally required for GVL formation. So far, the hydrogenation of levulinic acids/esters under mild conditions remains a great challenge. In this study, 2 wt.% Ru was loaded onto ZSM-5 zeolite (MFI) via a deposition–precipitation method and further wrapped by crystallization, forming a core–shell structure. Moreover, the wrapped Ru catalyst was coated with a petal-like layer of Mg3Si4O9(OH)4(MgSiO3) via a hydrothermal reaction in a Mg(NO3)2solution, thereby introducing alkalinity and achieving spatial separation of Mg and Ru. This dual-functional catalyst reduces the inhibitory effect of Mg on the Ru active center and enables efficient preparation of GVL from ethyl levulinate (EL) under mild conditions, achieving 100% EL conversion and 98% GVL selectivity in the aqueous phase at 80 °C in 2 h under 0.5 MPa of H2.
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高影响因子
Nanoscale
·
2026
·
IF 5.2
Jianbo Jiao,Jianfeng Lan,Guizhen Lu,Zhihui Ou,Jianhui Li,Yifei Sun,Li Zhang,Yanling Yang,Bo Wu,JianHua Wu
Titanium-based metal oxide anodes exhibit strong application potential in chlorine evolution antifouling systems from seawater electrolysis. Conventional dimensionally stable anodes (DSA) rely primarily on Ru- and Ir-based noble metal coatings, yet their large-scale industrial application is hindered by high costs and poor chlorine production efficiency. To overcome the aforementioned shortcomings, Co is introduced into the RuIrTiOx/Ti system, adopting a preparation process involving oxalic acid pretreatment and multi-step coating to fabricate RuIrCoTiOx/Ti electrodes. XRD and TEM results indicate a solid solution coating with uniformly dispersed elements formed on the electrode. The RuIrCoTiOx/Ti electrode demonstrates superior catalytic activity and nearly 84.4% faraday efficiency derived from the chlorine evolution compared to binary or ternary metal oxide-coated counterparts. Remarkably, the electrode maintains over 98.1% of its initial activity after 200 hours of continuous electrolysis. While the slightly reduced durability of RuIrCoTiOx/Ti compared to RuIrTiOx/Ti may be caused by an increased specific surface area of the mixed oxide coating and the formation of higher valence states of Ru species after Co incorporation, as evidenced by SEM and XPS results. This study provides an effective design strategy for developing low-cost, high efficiency DSA electrodes, offering promising prospects for industrial application.
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DOI
PubMed
高影响因子
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