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Catalysts · 2017 ·Vol. 7 ·期 10 ·311 · IF 3.082

Activated Carbon-Supported Tetrapropylammonium Perruthenate Catalysts for Acetylene Hydrochlorination

Xing Li,Haiyang Zhang,Baochang Man,Lijuan Hou,Chuanming Zhang,Hui Dai,Mingyuan Zhu,Bin Dai,Yanzhao Dong,Jinli Zhang

The Ru-based catalysts, including Ru/AC (activated carbon), TPAP (tetrapropylammonium perruthenate)/AC, TPAP/AC-HNO3, and TPAP/AC-HCl, were prepared and assessed for the direct synthesis of vinyl chloride monomer. The results indicate that the TPAP/AC-HCl catalyst exhibits the best performance with the conversion falling from 97% to 91% in 48 hours’ reaction under the conditions of 180 °C, a GHSV(C2H2) of 180 h−1, and the feed ratioVHCl/VC2H2of 1.15. The substitution of RuCl3precursor with high valent TPAP species leads to more ruthenium oxides active species in the catalysts; the acidification treatment of carrier in TPAP/AC catalyst can produce an enhanced interaction between the active species and the modified functional groups on the carrier, and it is beneficial to inhibit the carbon deposition and sintering of ruthenium species in the reaction process, greatly increase the adsorption ability of reactants, and further increase the amount of dominating active species in the catalysts, thus improving the catalytic performance. This also provides a promising strategy to explore high efficient and economic mercury-free catalysts for the hydrochlorination of acetylene.Keywords:tetrapropylammonium perruthenate;acetylene hydrochlorination;Ru catalysts

研究领域: 催化化学 · 环境科学 · 材料科学
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APPLIED SURFACE SCIENCE · 2023 · IF 6.7

Exceptionally active and stable RuO2 by constructing p-n heterojunction between Co3O4 and RuO2 for acidic water oxidation

Feng Zhou,Jiadong Chen,Yun Yang,Xiaofeng Ke,Xue Liu,Lijie Zhang,Jun Li,Huile Jin,Shun Wang,Ying Li,Chenliang Su

Development of Ru-based electrocatalysts for acidic oxygen evolution reaction without a trade-off between activity and durability remains challenging. Herein, we constructed Co 3 O 4 /RuO 2 heterojunctions anchored on carbon (Co 3 O 4 /RuO 2 -C) with a low Ru loading (2.74 wt%), in which strong coupled p-n junctions facilitated electron transfer from RuO 2 to Co 3 O 4 . The Co 3 O 4 /RuO 2 -C demonstrated a low overpotential of 170 mV at 10 mA cm −2 and long-term stability in 0.1 M HClO 4 due to its unique structure. The origin of its high performance in acidic OER was revealed by the combination of in-situ attenuated total reflection infrared and Raman tests. Concretely, oxygen generation for Co 3 O 4 /RuO 2 -C was dominated by the adsorbate evolution mechanism, and the introduction of Co 3 O 4 facilitated the redox of RuO 2 , generating active sites for OER. Theoretical calculations further substantiated that the Co 3 O 4 /RuO 2 heterojunctions possessed lower energy barriers for OER. This work provides a compelling synthesis route for effective and stable electrocatalysts for acidic OER.

研究领域: 材料科学 · 电化学 · 催化科学
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Journal of Materials Chemistry A · 2024 · IF 10.7

Reducing the hydrogen transfer barrier by the introduction of Ru via a constructed Ir–Ru–WO2.72 bridge for highly CO-tolerant hydrogen oxidation

Xu Yu,Han Tian,Ziyi Yu,Fantao Kong,Chang Chen,Ziwei Chang,Jian Huang,Xiangzhi Cui,Jianlin Shi

Hydrogen spillover effect-based active catalyst design is an effective strategy to enhance the hydrogen oxidation reaction (HOR) performance, which, unfortunately, still suffers from the high hydrogen spillover energy barrier. Here, a strategy alloying Ir with Ru is proposed to modulate the electronic structure of Ir to accelerate the H* transfer by a novel Ir–Ru–WO2.72 bridge, thus significantly reducing the hydrogen spillover energy barrier from Ir to WO2.72. The IrRu nanoclusters were deposited on a three-dimensional ordered macroporous WO2.72–C framework, and thus the constructed IrRu–WO2.72–C (1.16 wt% Ir and 1.09 wt% Ru) catalyst exhibits excellent HOR and CO-tolerance performance, rather high cell power density, and especially, 4 times higher mass activity than that of Pt/C. The modulation of Ru largely decreases the work function difference between the IrRu clusters and substrate, resulting in a reduced hydrogen spillover barrier via the Ir–Ru–WO2.72 bridge, weakened CO adsorption and fast removal of the adsorbed CO.

研究领域: 材料科学 · 催化化学
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Biochar · 2022 ·Vol. 4 ·期 1 ·1-13 · IF 11.452

Biochar aerogel-based electrocatalyst towards efficient oxygen evolution in acidic media

Hui Bin,Chen Hongjiao,Zhou Chengfeng,Cai Liping,Zhang Kewei,Quan Fengyu,Yang Dongjiang

The controllable synthesis of oxygen evolution reaction (OER) electrocatalyst is an urgent need to advance the development of sustainable energy conversion and storage. However, the OER efficiency in acidic media is seriously hindered by slow reaction kinetics. The traditional acidic OER electrocatalysts are more prone to be oxidized and corroded as results of unstable carrier structures and variable electronic states of active species. Herein, a high-performing biochar aerogel (BA) based electrocatalyst were realistically designed and synthetized via joint utilization of the terrestrial lignin and seaweed polysaccharide as carbon sources.  Originating from the induction effect of "egg-box" structure in alginate and the self-template effect of lignosulfonate, the BA decorated with Ru/RuS 2 particles was synthesized triumphantly. The as-synthesized electrocatalyst required a low overpotential of 228 mV to attain 10 mA cm −2 in 0.5 M H 2 SO 4 and exhibited a good stability for over 12,000 s. The good activity was strongly dependent on the assembled unique two-dimensional/three-dimensional (2D/3D) channels in carbon aerogels. Notably, the numerous defective sites at carbon could strongly interact with the Ru/RuS 2 heterojunction for remarkably enhancing the catalytic activity and stability of whole catalytic system in acidic media. This work puts  forward a novel and effective strategy towards the enhancement of the acidic OER process by rational regulations of the BA and the coupling effect in micro-interface. Graphical Abstract

CAS / MDL: 10049-08-8 8061-51-6
研究领域: 材料科学 · 电化学 · 可再生能源
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ELECTROCHIMICA ACTA · 2023 · IF 6.6

Valence regulation of Ru/Mo2C heterojunction for efficient acidic overall water splitting

Zhao Liu,Yuxuan Liu,Huawei He,Hongbo Shao,Yi Zhang,Jing Li,Weiwei Cai

Hydrogen production by water splitting has the characteristics of clean, efficient, and strong operability. However, it is limited by the low activity and insufficient stability of cathode and anode catalysts. Therefore, cost-effective catalysts for efficient cathodic hydrogen evolution reaction (HER) and anodic oxygen evolution reaction (OER) have to be developed. In this work, Ru/Mo 2 C heterojunctions are constructed to regulate the valence of Ru and Mo in the catalyst to simultaneously boost HER and OER in acidic conditions. Consequently, the overpotentials providing 10 mA/cm 2 HER and OER in the acidic electrolyte are reduced to 40 mV and 215 mV, respectively. Finally, only 1.51 V applied voltage is required to achieve 10 mA/cm 2 acidic overall water splitting. Taking stability into consideration, the Ru/Mo 2 C catalyst shows good application prospects in practical acid water electrolysis devices.

研究领域: 材料科学 · 能源化学
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ADVANCED FUNCTIONAL MATERIALS · 2025 · IF 19

Electron-Rich Ru Atoms in Loaded Ru4Fe Intermetallic Compounds/C Modulate the Kinetics of Neutral Hydrogen Evolution

Wen Zhang,Guang-Rui Xu,Tiantian Sun,Jiayi Li,Yu Miao,Zexing Wu,Yang Zhang,Lei Wang

Intermetallic compounds (IMCs) with long-range atomic-scale ordering are an emerging class of efficient and stable electrocatalytic alloy materials. Compared with disordered alloys, IMCs show a better electronic structure and higher mixing enthalpy. Herein, the ordered Ru 4 Fe intermetallic compounds with a diameter of 15 nm on porous carbon (Ru 4 Fe IMCs/C) are synthesized by a sol–gel and annealing steps, the interaction of Ru 4d and Fe 3d orbitals produces an anisotropic electron distribution, which facilitates the adsorption of water molecules and accelerates their dissociation, which exhibit excellent hydrogen evolution at all pH values. At the current density of 10 mA cm −2 , the overpotentials of Ru 4 Fe IMCs/C are 29, 24, and 36 mV in acidic, neutral, and alkaline media for hydrogen evolution reaction (HER), respectively, superior to that of Pt/C catalysts with a mass loading of 20%. Mechanistic studies suggest that the adsorption Gibbs free energy of *H (ΔG *H ) on Ru 4 Fe IMCs/C is closer to 0 eV compared to Ru NPs/C, which facilitates the HER process.

研究领域: 材料科学 · 电催化
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ChemCatChem · 2022 ·Vol. 14 ·期 24 ·e202201010 · IF 5.497

Ru−RuO2 Nanoparticles Decorated on Various Substrates via Reduction-Hydrolysis Strategy for Boosting Overall Water-Splitting Performance

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.

CAS / MDL: 14898-67-0
研究领域: 材料科学 · 电化学 · 纳米技术
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Journal of Materials Chemistry A · 2024 · IF 10.7

The critical role of Ru-like hydrogen adsorption of carbon dots in a carbon-confined Ru system for boosted HER activity

Zonglin Liu,Honglei Zhang,Dongyue Liu,Yujie Feng,Dechang Jia,Caicai Li,Qingfeng Sun,Yu Zhou,Zhenhui Kang,Baoqiang Li

The in-depth understanding of electrocatalysts is the key issue in the fields of clean energy and the chemical industry. Although various carbon-loaded active metal particle catalysts for the electrocatalytic hydrogen evolution reaction (HER) have been developed, the interaction between active metals and the substrate is still unclear. Herein, ruthenium (Ru) nanoparticles loaded on N-doped carbon dots (Ru/NCDs) were constructed to discover the critical roles of the carbon substrate as well as its interaction with Ru. Notably, we show the two critical functions of NCDs in a carbon-confined Ru system. First, the ultra-small Ru nanoparticles increase the hydrogen spillover channels. Second, the carbon substrate shows a Ru-like hydrogen adsorption capacity, supplying sufficient H sources for hydrogen spillover. Thus, the hydrogen spillover is enhanced and the HER process is accelerated. The Ru/NCDs catalyst shows superior HER activity and durability in both acidic and alkaline solutions. This work clarifies the critical role of carbon substrates in carbon-loaded catalysts.

CAS / MDL: 9012-76-4 108-78-1
研究领域: 电化学 · 催化 · 清洁能源 · 材料科学
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CRYSTENGCOMM · 2023 ·Vol. 25 ·期 6 ·981-987 · IF 3.1

Anchored RuSe2 nanospheres on Co–N–C nanosheets boost electrocatalytic alkaline hydrogen evolution

Nan Li,Minghao Shi,Wei Zhan,Wenjing Shen,Mianmian Wu,Guifang Sun,Qingfei Li,Jiangquan Ma

Ru-based catalysts are potential substitutes for Pt in the hydrogen evolution reaction (HER). It is worth noting that the Se ions in RuSe2 can modulate the electronic structure of the Ru metal, thus effectively improving the HER kinetics of RuSe2. However, single electronic structure modulation is hard to complete due to the electron deficiency of active Ru atoms. Herein, we prepare and design a novel RuSe2/Co–N–C (RuSe2 nanospheres supported on Co–N–C nanosheets) electrocatalyst with two-electron modulation by a hydrothermal and thermal annealing method. Benefiting from the uniform distribution of RuSe2 nanospheres on Co–N–C nanosheets and Co–N–C nanosheets acting as additional electron donors to make up for the electron deficiency of the Ru metal, RuSe2/Co–N–C exhibits excellent HER performance with a low overpotential of 26.4 mV at 10 mA cm−2 and a low Tafel slope of 53.2 mV dec−1. This work offers an effective method for the synthesis of high catalytic performance electrocatalysts by constructing an interaction between the carrier and the active metal.

研究领域: 材料科学 · 电化学
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RSC Advances · 2014 ·Vol. 4 ·期 94 ·52402-52409 · IF 3.708

Direct conversion of cellulose into C6 alditols over Ru/C combined with H+-released boron phosphate in an aqueous phase

Yong Liu,Lungang Chen,Tiejun Wang,Ying Xu,Qi Zhang,Longlong Ma,Yuhe Liao,Ning Shi

Non-edible cellulose has attracted considerable attention to be converted into valuable platform chemicals. Direct transformation of cellulose to C6 alditols (mannitol and sorbitol) provides a sustainable route. A productive approach is presented in this work using a Ru/C catalyst combined with H+-released boron phosphate in an aqueous phase. A yield of C6 alditols as high as 74.9% with a 91% conversion of cellulose is achieved. By adding silica–alumina materials, the yield of C6 alditols can be improved to 93.5% with complete conversion. The acid sites gradually released from boron phosphate under hydrothermal conditions could promote the hydrolysis of cellulose without significant degradation of glucose. Furthermore, the interaction of boric acid with C6 alditols may form borate–polyol complexes, which can enhance the stability of the C6 alditols to avoid further hydrogenolysis and dehydration of the C6 alditols formed. Due to the adsorption ability of the substrate, the addition of silica–alumina materials with a high content of silica leads to improved performance.

CAS / MDL: 7440-18-8 12027-43-9
研究领域: 化学工程 · 可再生资源利用
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JOURNAL OF ALLOYS AND COMPOUNDS · 2024 · IF 5.8

Anchoring Ru-Ru2P heterojunction on P-doped graphene for enhanced HER performances of water electrolysis

Longyang Liu,Zichen Wang,Xueyan Zhang,Lijie Luo,Yongjun Chen

Highly active and stable electrocatalysts are highly desired for the hydrogen evolution reaction (HER) in water electrolysis. In this study, a ruthenium-ruthenium phosphide heterojunction (Ru-Ru 2 P) anchored on phosphorus-doped graphene (PCSG) was fabricated via a mild molten salt template method. The graphene was synthesized from discarded coconut shells sourced from Hainan. We found that the heterojunction structure could accelerate electron transfer, while the graphene provided more exposed active sites, significantly enhancing the HER activity of the catalyst. The catalyst prepared at 800 °C with 30 mg of RuCl 3 (Ru-Ru 2 P/2D-PCSG-800) exhibited low HER overpotentials of 31 mV in alkaline and 57 mV in acidic electrolytes at a current density of 10 mA cm −2 , respectively, which were comparable to those of commercial 20 % Pt/C catalyst (36 mV in alkaline and 40 mV in acidic electrolytes). Moreover, the catalyst demonstrated high stability with no significant change in current density after 125 hours of operation. Density functional theory calculations revealed that the Ru-Ru 2 P heterojunction could rearrange charge and modify the Ru d -band center, optimizing the adsorption energy of active *H (|ΔG *H |) and breakage energy of *H-OH bond (ΔG H2O ).

研究领域: 材料科学 · 电化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Ruthenium–molybdenum nanoparticles with multi-valence ruthenium species to drive redox electrocatalysis at high current densities

Shuanglong Zhou,Liang Zhao,Yuanduo Li,Hangkai Shi,Weizhou Wang,Yu Dai,Jianping Lai,Lei Wang

Coupling furfural electrochemical hydrogenation (FEH) with hydrazine oxidation (HzOR) in an electrochemical process offers an effective pathway to obtain high-value products, while simultaneously addressing hydrazine contamination and lowering overall energy consumption. Although Ru has been recognized as an effective bifunctional catalyst toward both FEH and HzOR, challenges remain in achieving large current densities and fully clarifying the underlying activity and mechanism. In this work, a Ru-based device was engineered by introducing Mo dopants to regulate the proportion of Ru 0 and Ru 4+ species, which enabled a remarkable current density of 500 mA cm −2 at 0.31 V. Combined experimental and theoretical investigations demonstrate that Ru 0 sites enhance water dissociation to generate active hydrogen for subsequent hydrogenation, while Ru 4+ sites stabilize the (C 4 H 3 O)CH 2 O* intermediate during FEH. For HzOR, Ru 4+ lowers the barrier of the rate-determining step, thus accelerating the overall process, whereas Ru 0 facilitates dehydrogenation and the release of N 2 . Notably, the integrated FEH–HzOR system dramatically reduces the electricity demand for converting furfural to furfuryl alcohol, requiring only 32,711 kWh per ton of FA, which corresponds to a 69.5 % energy saving compared with conventional FEH (97,766 kWh per ton).

研究领域: 电化学 · 纳米催化 · 能源化学 · 环境催化 · 绿色合成
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