JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Xinyu Guo,Jiaxin Li,Fanze Meng,Dongdong Qin,Xueyan Wu,Yan Lv,Jixi Guo
Properly design and manufacture of bifunctional electrocatalysts with superb performance and endurance are crucial for overall water splitting. The interfacial engineering strategy is acknowledged as a promising approach to enhance catalytic performance of overall water splitting catalysts. Herein, the Ru nanoparticles modified Ni 3 Se 4 /Ni(OH) 2 heterostructured nanosheets catalyst was constructed using a simple two-step hydrothermal process. The experimental results demonstrate that the abundant heterointerfaces between Ru and Ni 3 Se 4 /Ni(OH) 2 can increase the number of active sites and effectively regulate the electronic structure, greatly accelerating the kinetics of the hydrogen evolution reaction (HER)/oxygen evolution reaction (OER). As a result, the Ru/Ni 3 Se 4 /Ni(OH) 2 /NF catalyst exhibits the low overpotential of 102.8 mV and 334.5 mV at 100 mA cm −2 for HER and OER in alkaline medium, respectively. Furthermore, a two-electrode system composed of the Ru/Ni 3 Se 4 /Ni(OH) 2 /NF requires a battery voltage of just 1.51 V at 10 mA cm −2 and remains stable for 200 h at 500 mA cm −2 . This work provides an effective strategy for constructing Ru-based heterostructured catalysts with excellent catalytic activity.
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FUEL PROCESSING TECHNOLOGY
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2024
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IF 7.2
Yucan He,Dongsen Mao,Qiangsheng Guo,Jun Yu
A series of highly ordered microporous Ce-based metal-organic frameworks (MOFs) were synthesized as the precursors for catalyst construction. The corresponding Ru catalysts were prepared by Ru impregnation on the derived CeO 2 by pyrolysis of Ce-MOF, and investigated for the CH 4 synthesis via CO 2 hydrogenation. Among the catalysts, Ru catalyst supported on the CeO 2 -B derived from Ce-BDC exhibited a highly competitive efficiency for CO 2 methanation, giving a CH 4 selectivity of 100% with a CO 2 conversion of 62% at 275 °C and 0.1 MPa, and the CH 4 productivity reached 0.49 mol/(mol Ru ·h). Characterization results revealed that more oxygen vacancies and corresponding surface oxygen species formed on the surface of CeO 2 -B derived from Ce-BDC caused to the stronger interaction between Ru and CeO 2 -B, which promoted the CO 2 adsorption and hydrogenation capacity of the catalyst, resulting in its better catalytic property. In situ diffuse reflectance infrared Fourier transform (DRIFT) studies further revealed that the route of HCOO* into CH 4 is a more competitive way of CO 2 hydrogenation to CH 4 .
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
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IF 20.2
Yan Liu,Liwen Xing,Yaqi Liu,Dianxing Lian,Mohaoyang Chen,Weiwei Zhang,Ke Wu,Hongdan Zhu,Zhiyi Sun,Wenxing Chen,Peng Wu,Dingsheng Wang,Yongjun Ji
The intrinsic activity of single-atom catalysts is influenced by the local electronic structures of metal centers, with existing modulation strategies limited to adjacent atomic coordination. However, the impacts of support surface geometry on local bonding environment, and thus electronic structures of single-atom centers have rarely been known. Here, we prepared highly curved B,N co-doped carbon-supported ruthenium catalyst with an ultra-low Ru loading of 0.4 wt%, which exhibited an ultrahigh turnover frequency (TOF) of 10 H 2 s −1 (38 times that of Pt/C) and superior stability in alkaline hydrogen evolution reaction (HER). We found that curving support surface induced the strain, resulting in 1.5% compressed Ru-N and 4% stretched Ru-B bonds, leading to the accumulation of positive charge and quenching of spin polarization at Ru sites, thereby achieving the optimal binding of H* and enhanced performance for HER. This work highlights the significant support effects upon the structural design of active sites.
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ADVANCED MATERIALS
·
2024
·Vol. 36
·期 33
·2400433
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IF 27.4
Chaohui Wang,Jun Zhang,Kanghua Miao,Mairui Long,Siyuan Lai,Shijun Zhao,Xiongwu Kang
Integrating high-entropy philosophy and nanocrystal-specific orientation into a single catalyst represents a promising strategy in development of high-performance catalysts. Nonetheless, shape-controlled synthesis of high-entropy alloy (HEA) nanocrystals is challenging owing to the distinct redox potentials and growth dynamics of metal elements. Herein, a one-pot co-reduction method is developed to fabricate ruthenium (Ru)-doped PtFeNiCuW octahedral HEA nanocrystals onto carbon nanotubes (Ru–PtFeNiCuW/CNTs). It is demonstrated that Ru dopants and W(CO) 6 promote the concurrent reduction and growth of other metal precursors to obtain higher yield and larger size of HEA nanocrystals, despite low Ru content in Ru–PtFeNiCuW/CNTs. As an electrocatalyst toward hydrogen evolution reaction (HER), Ru–PtFeNiCuW/CNTs exhibits low overpotentials of 9, 16, and 34 mV at a current density of 10 mA cm −2 and Tafel slopes of 19.2, 27.9, and 23.1 mV dec −1 in acidic, alkaline, and neutral electrolytes, respectively. As a cathodic catalyst, Ru–PtFeNiCuW/CNTs operates for up to 1500 and 1200 h in acidic and alkaline electrolyte, respectively, at a current density of 50 mA cm −2 in a two-electrode system for full water splitting. Theoretical calculations reveal accelerated kinetics of H 2 O dissociation on W sites and *H desorption on hollow Cu–Cu–Cu and Cu–Cu–Pt sites.
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ADVANCED MATERIALS
·
2025
·
IF 26.8
Hang Wang,Han Xu,Fei Yang,Yan Qing,Fuxiang Chu,Yiqiang Wu,Sheng Ye,Fuquan Xiong
Local electric fields of the electrocatalysts can modulate adsorbate binding energies based on their polarizability and dipole moment, which directly influence the catalytic performance. Nevertheless, implementing the prevailing strategy remains challenging due to the scarcity of active sites and sluggish catalytic kinetics. Herein, a continuous heterogeneous-curvature nanoreactor (HeterC-LCS) is created to enhance local electric fields by optimizing the uniform-nanocurvature with tip effects. The H + concentration and H 2 O transmission rate of HeterC-LCS are improved by about 2.1 and 1.7 times that of the homogeneous curvature structure (HomoC-LCS) during the hydrogen evolution reaction (HER) process. Besides, HeterC-LCS demonstrates a rapid kinetics of intermediate transformation and an extremely low energy barrier. Such HeterC-LCS depicts a lowest overpotential of 9.2 mV at 10 mA cm −2 , which outperforms all known carbon- and Ru-based electrocatalysts. And the mass activity is approximately 60 times that of commercial Pt/C. This work proposes a novel strategy of uniform-nanocurvature optimized by tip effects toward industrially electrocatalytic HER.
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ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Huan Chen,Qian Yang,Jixiang Li,Jiangyong Li,Wenjing Hu,Liangke Zhang
Cell organelle-based tumor-targeting strategies offer more precise approaches for tumor treatment, reducing adverse reactions and drug dosage. Mitochondria play a crucial role in cell proliferation and signal transduction, making them important organelle targets for disease intervention. This study developed a novel mitochondria-targeting and ultrasound-responsive nanosystem (MRTP) that can control the release of reactive oxygen species (ROS) and carbon monoxide (CO). MRTP is a combination of narrow-band gap sonosensitizers and mitochondria-targeting CO-releasing molecules. It can effectively cross both cellular and mitochondrial barriers and selectively target tumor cell mitochondria. When ultrasound is focused on the tumor site, MRTP can precisely release ROS and CO. Interestingly, MRTP can improve the tumor microenvironment (TME), not only alleviating tumor hypoxia but also depleting glutathione and catalyzing the generation of ·OH from H2O2. These TME regulatory strategies can increase the level of ROS production. Ultimately, the cascade effect of ROS and CO generation will reduce mitochondrial membrane potential, promote tumor cell apoptosis, and inhibit tumor growth.
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ACTA MATERIALIA
·
2025
·
IF 9.3
Xianqiang Yu,Yuezhu Wang,Mingze Xia,Li Deng,Ruikai Qi,Mingbin Gao,Mengxiao Zhong,Xiaofeng Lu
Manipulating the electronic structure of heterogeneous catalysts to optimize the adsorption behavior of hydrogen intermediate (H*) is essential for enhancing the hydrogen evolution reaction (HER), representing a key objective in advancing efficient hydrogen (H 2 ) production. Herein, we have engineered the electronic configuration by coupling ruthenium (Ru) nanoparticles with molybdenum carbide (Mo 2 C)/N-doped carbon fibers (NCF) to greatly enhance the electrocatalytic alkaline/acidic-universal HER performance. The obtained Ru@Mo 2 C/NCF catalyst exhibits ultralow overpotentials of 182 and 193 mV at an industrial-grade current density (1 A cm⁻ 2 ) in 1 M KOH and 0.5 M H 2 SO 4 , respectively, significantly surpassing commercial Pt/C and many traditional HER catalysts. The catalyst also demonstrates an exceptional long-term stability in both alkaline and acidic conditions, even greatly better than Pt/C catalyst. Theoretical analysis reveals that the coupling of Ru with Mo 2 C/NCF optimize the H* adsorption and facilitates H 2 releasing. Furthermore, a zinc-water (Zn-H 2 O) battery is assembled to realize highly efficient and simultaneous H 2 and electricity generation, demonstrating its practicability.
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ChemSusChem
·
2024
·
IF 7.5
Tao Yin,Yichao Ye,Hao Jiang,Chengyin Lin,Riyang Shu,Zhipeng Tian,Chao Wang,Ning Shi
Graphical This work proposed a novel and stable Ru-based catalyst with biochar and Al 2 O 3 as composite support, which achieved an outstanding performance on the hydrodeoxygenation of lignin-derived phenolic compounds and raw lignin-oil. Under the catalysis of optimized Ru/C-Al 2 O 3 catalyst, the hydrocarbon content increased significantly from 10.7 % to 95.7 % at 230 °C. Hydrodeoxygenation (HDO) is a common strategy for upgrading lignin-derived phenolic compounds into high-quality liquid fuels, and the support rational design of HDO catalysts is critical to achieve a good reaction performance. This work proposed a novel Ru-based catalyst with biochar and Al 2 O 3 as composite support. The addition of biochar can enlarge the porous structure, and the addition of Al 2 O 3 can enhance the acid property of the support. By regulating the content of biochar and Al 2 O 3 components, Ru/CA-2 catalyst achieved the best HDO performance of lignin-derived phenolic compounds, with the optimal component balance of 50 %C and 50 %Al 2 O 3 . This catalyst possesses the high Ru metal dispersion (1.38 nm particle size) to activate the hydrogen source, the moderate acid property to suppress carbon deposition and the abundant oxygen vacancy to promote substrate adsorption at the same time. 99.9 % conversion of guaiacol is obtained at 230 °C, with 99.9 % selectivity towards cyclohexane. Ru/CA-2 catalyst also has a good recyclability, with no obvious activity loss after five runs. Furthermore, in the application of catalytic lignin-oil HDO, the content of hydrocarbons increase from 10.7 % to 95.7 %, showing great potential on the industrial usage.
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CHEMICAL ENGINEERING JOURNAL
·
2025
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IF 13.2
Qihao Wang,Yusen Chen,Xingchao Zang,Hongdong Li,Weiping Xiao,Yingxia Zong,Guangying Fu,Jinsong Wang,Zexing Wu,Lei Wang
A breakdown of the Sabatier principle is essential for the substantial improvement of the catalytic performance of the hydrogen evolution reaction (HER). This can be achieved by alternating the support and electronic metal support interaction (EMSI). Herein, ZrO 2 supported Ru and Pt (Pt-Ru/ZrO 2 ) with EMSI is designed through ultrafast microwave-plasma (60 s) approach. Pt-Ru/ZrO 2 requires only 33 mV overpotential to reach 10 mA cm −2 in alkaline HER, which is 6.3 times the mass activity of the benchmark Pt/C. HER performance is enhanced in the presence of EMSI because it optimizes the hydrogen adsorption and desorption processes, improves charge transfer and improves the kinetics of water dissociation. In addition, the assembled anion exchange membrane (AEM) electrolysis cell maintains long-term stability for more than 150 h at 1 A cm −2 , demonstrating a sustained catalytic effect. This work offers a novel design approach for developing electrocatalysts with remarkable performance when subjected to high-current–density conditions of industrial scenarios
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-14
·
IF 15.7
Wang Peng,Zhao Danyang,Zhang Peng,Hui Xiaobin,Zhang Zhiwei,Wang Rutao,Wang Chengxiang,Ge Xiaoli,Liu Xiaojing,Li Yuguang C.,Yin Longwei
The metallic phase MoS 2 (1T-MoS 2 ) supported metal-nanocatalyst is an appealing material system for accelerating the redox kinetics of non-aqueous Li | |O 2 batteries. However, the drawbacks associated with the surface orbital steric effect and the internal electron coupling results in a detrimental effect for the stability of 1T-MoS 2 , especially for the interface charge transfer. This makes it difficult to incorporate guest metal nanoparticles without compromising the 1 T phase support. To circumvent these issues, here we propose a p-block element (In-O) doping strategy to stabilize the 1 T phase MoS 2 by moderating the surface orbital steric effect and strengthening the internal chemical bonding, and thus for the epitaxial Ru nanocatalyst graft on the stabilized 1T-MoS 2 for Li | |O 2 batteries. The experimental and theoretical analyzes indicate that the In-O-MoS 2 @Ru enhances the O 2 dissociation and facilitates the adsorption of LiO 2 intermediates. This effect promotes the growth of weakly crystalline Li 2 O 2 films during oxygen reduction reaction, which can be more easily decomposed during the oxygen evolution reaction, thereby enhancing the bifunctional-catalytic kinetics. When employed at the positive electrode for non-aqueous Li | |O 2 batteries, In-O-MoS 2 @Ru shows an overpotential of 0.37 V and a cycling life of 284 cycles at 200 mA g −1 with a final discharge specific capacity of 1000 mAh g −1 at 25 °C.
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Yuhao Zhang,Luting Yan,Lei Tian,Qi Guo,Maosheng Sang,Shouyi Dou,Falan Li,Qingqing Yang,Xia Sun,Yemin Guo,Yanyan Zhang
Vibrio parahaemolyticus ( VP ) is one of the most common pathogens in aquatic products, and its study using electrochemiluminescence is still relatively rare. In this study, an electrochemiluminescent (ECL) biosensor was developed to detect VP in aquatic products using AuNPs modified PEI/MWCNTs (AuNPs@PEI/MWCNTs) as a substrate material and ordered mesoporous carbon (OMC) adsorbed Ru(bpy) 3 2+ (OMC@Ru(bpy) 3 2+ ) as a luminescent material. To increase the conductivity of the biosensor and offer a favorable loading environment for the immobilization of the luminescent probe, AuNPs@PEI/MWCNTs are employed as the substrate. Meanwhile, the OMC@Ru(bpy) 3 2+ functionalized DNA probe acts as a luminescent and capture probe to generate ECL signals and specifically recognize different concentrations of VP . The biosensor has good selectivity and stability and has been successfully applied to the detection of VP in scallops. This method not only expands the potential uses of bioprobe-based ECL biosensors, but also offers a new and effective approach used to detect food-borne pathogens in aquatic products.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Yu-Xuan Fu,Shu-Yi Huang,Ming-Shuai Sun,Yan Zhou,Dan-Dan Cai,Wen-Shuai Zhu,Wei Hui,Duan-Jian Tao
Current industrial catalysts for α-pinene hydrogenation suffer from harsh reaction conditions and poor selectivity to cis -pinane, primarily due to their inability to effectively adsorb α-pinene in a specific favorable configuration on the catalyst surface. In this study, a high-specific-surface-area, rod-shaped CeO 2 -supported ultra-fine Ru nanoparticle (average particle size of 4 nm) catalyst was synthesized via hydrothermal method for the highly stereoselective hydrogenation of α-pinene to cis -pinane. The resulting Ru/CeO 2 -H catalyst achieved an α-pinene conversion of 99.3 % and an impressive cis -pinane selectivity of up to 99.6 % under exceptionally low temperature (30°C), 0.6 MPa H 2 and 0.5 h with high TOF (1236 h −1 ). Density functional theory (DFT) calculations indicated that α-pinene preferentially adsorbs onto the Ru surface via the backside of its intramolecular dimethyl bridge. This particular adsorption mode lowers the energy barriers for further hydrogenation to generate cis -pinane. The oriented dimethyl-up configuration of α-pinene and ultra-low activation energy (12.04 kJ/mol obtained from kinetic tests) enable the highly selective production of cis -pinane at ambient temperature. Furthermore, the strong interaction between the CeO 2 -H support and highly dispersed Ru, combined with the ambient-temperature reaction conditions, effectively prevents metal nanoparticle agglomeration and coking, imparting the catalyst with exceptional stability. Notably, the catalyst was reused at least 15 times without observing any significant deactivation, demonstrating its significant potential for practical applications.
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