JOURNAL OF MEDICINAL CHEMISTRY
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2024
·
IF 6.8
Zhongyu Wang,Li Wei,Junfeng Lin,Can Huang,Huitong Chen,Dong Fan,Weiyu Hu,Jing Liu,Huaiyi Huang,Zongming Wang,Xin Wang
Photodynamic therapy has been regarded as a noninvasive treatment for cancer with spatiotemporal control over drug activation. Bis-terpyridyl Ru(II) complexes exhibit a promising achiral structure but suffer from low photoreactivity due to deviation from the ideal octahedral geometry. Herein, we introduce the donor–acceptor–donor motif to construct a dinuclear bis-terpyridyl Ru(II) complex (Ru2). Ru2 exhibits superior light absorption properties compared with mononuclear complex Ru1. Importantly, upon 595 nm light excitation, Ru2 shows promising synergetic type I/II photosensitization and photocatalytic activity, while Ru1 is inactive. Anticancer mechanistic studies reflect that Ru2 induces intracellular redox imbalance and affects the biosynthetic and metabolic processes, leading to cell apoptosis. Overall, this work provides a simple strategy to rouse the PDT efficiency of bis-terpyridyl Ru(II) complexes.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2024
·
IF 20.2
Yue Shi,Jiawei Fei,Hongdong Li,Caixia Li,Tianrong Zhan,Jianping Lai,Lei Wang
Amorphous metallene is a prospective catalyst due to disordered atomic arrangement and abundant defects/edges. However, challenges persist in preparing amorphous metallene with atomic interface, primarily due to thermodynamic impediment of unconventional phase and difficulty in precise controlling of atomic interface. Here, we synthesized a new class of amorphous RuGa metallene (A-RuGa metallene) with abundant atomic interface by introducing trace atomic-dispersed Ga. The atomic interface between Ga-coordinated Ru and Ru 0 achieves monometallic synergism during alkaline hydrogen evolution reaction. The turnover frequency value of A-RuGa 0.06 metallene reaches 67 s −1 at −0.1 V vs. RHE. Meanwhile, the mass activity of A-RuGa 0.06 metallene in anion exchange membrane electrolyzer reaches 5.2 A mg Ru −1 at 2.0 V, firstly surpassing commercial Pt/C (1.0 A mg Pt −1 ). The trace atomic dispersed Ga could change the local valence state of monometallic Ru, thus promoting water adsorption and dissociation, optimizing H* adsorption and accelerating H* transport at the atomic level.
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Materials Chemistry Frontiers
·
2024
·Vol. 8
·期 14
·2592-2598
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IF 6
Jinfu Hou,Yongqi Jian,Chengjie Chen,Dengke Zhang,Fangyan Xie,Jian Chen,Yanshuo Jin,Nan Wang,Xiang Yu,Hui Meng
FeNC is a promising non-precious metal catalyst that can replace platinum-based catalysts in proton-exchange membrane fuel cells (PEMFCs) and zinc–air battery applications. The study utilized Fe-ZIF-8 as a precursor to improve the oxygen reduction reaction (ORR) activity of the catalyst. This was achieved by growing ruthenium particles of approximately 0.32 μm in situ using a physical milling method under a reducing gas atmosphere. This paper demonstrates that in situ grown ruthenium nanoparticles can alter the spin state of iron atoms from the high-spin state FeN4(II)-(t42ge2g) to the medium-spin state FeN4(II)-(t52ge1g). This alteration changes the interactions of the π* antibonding orbitals of the oxygen and thus improves the ORR activity. The rotating ring-disk (RDE) electrode test resulted in a half-wave potential of (E1/2) + 0.80 V vs. RHE in 0.1 M HClO4, indicating remarkable ORR performance. Zinc–air battery tests showed a high peak power density of 148 mW cm−2.
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Nanoscale
·
2024
·Vol. 16
·期 23
·11250-11261
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IF 5.8
Tingxia Wang,Xu Zhang,Xiaojiao Yu,Yun Liu,Junpeng Li,Zongbin Liu,Ningning Zhao,Jian Zhang,Jinfen Niu,Qingliang Feng
High-efficiency water electrolysis over a broad pH range is desirable but challenging. Herein, Ru-decorated VS2 on carbon cloth (Ru–VS2/CC) has been in situ synthesized, which features the regulated electronic structure of VS2 by introducing Ru. It is remarkable that the optimal Ru–VS2/CC displays excellent electrocatalytic hydrogen evolution activity with overpotentials of 89 and 87 mV at −10 mA cm−2 in 0.5 M H2SO4 and 1.0 M KOH, respectively. Theoretical calculations and electrocatalytic measurements have demonstrated that introducing Ru induces an enhanced charge density around the Fermi level, facilitating charge transfer and speeding up the electrocatalytic HER kinetics. The Gibbs free energy of the hydrogen intermediate (ΔGH*) of Ru–VS2/CC (0.23 eV) is much closer to zero than that of pure VS2 (0.51 eV) and Ru (−0.37 eV), demonstrating an easier hydrogen adsorption and desorption process for Ru–VS2/CC. The more favorable ΔGH*, differential charge density and the d-band center endow Ru–VS2 with enhanced intrinsic electrocatalytic activity. This study presents a feasible strategy for enhancing electrocatalytic HER activity by the regulation of the electronic structure and the rational integration of dual active components.
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JOURNAL OF POWER SOURCES
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2024
·
IF 8.1
Qi Ling,Kui Yan,Ziwei Zhao,Zihan Zhou,Zhaoqi Sun,Lei Yang,Miao Zhang
Due to the growing demand for clean renewable hydrogen fuel , the rational design of electrode materials' composition and structure holds significant importance in achieving efficient energy storage and conversion in electrochemical energy devices. In this study, we synthesize NiCo-MOF74/NF substrate using a one-step hydrothermal method , after which we successfully deposit a layer of Ru metal nanoclusters on the substrate by electrodeposition . Ru NCs@NiCo-MOF74/NF exhibits an exceptionally large specific surface area and excellent interface effects, demonstrating outstanding performance in both overall water splitting and supercapacitor applications. In a 1 M KOH alkaline solution, the device requires only 1.47 V output voltage to deliver a current density of 10 mA cm −2 for overall water splitting. As a supercapacitor , the unique nanoflower structure of Ru NCs@NiCo-MOF74/NF enables fast and reversible Faradaic reactions, providing high specific capacitance and rate performance. It shows a high areal capacitance of 1.664 mAh cm −2 at 1 mA cm −2 , indicating excellent charge storage capacity. Assembled into an asymmetric supercapacitor (ASC) with Ru NCs@NiCo-MOF74/NF as the positive electrode , the device achieves a high energy density of 511.88 μWh cm −2 at a power density of 545.68 μW cm −2 . After 5000 cycles, the capacitance retention rate is approximately 100 %, demonstrating remarkable cycling stability. This paves the way for the synthesis of multifunctional catalysts, opening up new possibilities in the field.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Yihan Zhang,Song Wu,Ting Sun,Qianggen Li,Guangyin Fan
The development of a rapid and convenient strategy to regulate the surface microenvironment of inert carbon supports, along with the physicochemical properties of their supported metal nanoparticles, is essential for enhancing catalytic performance. In this study, we describe a straightforward and efficient solid-state microwave method that utilizes a household microwave oven to achieve the co-doping of oxygen and nitrogen in unfunctionalized carbon black (ONCB) using urea as a nitrogen source. The microwave solid-state treatment of commercial carbon black (CB) with urea not only introduces a significant number of heteroatomic functional groups but also substantially increases the pore size and pore volume of the matrix. These enhancements facilitate the uniform growth and dispersion of ultrafine Ru nanoparticles on the surface of ONCB. Consequently, the Ru/ONCB catalyst provides abundant catalytic active sites and mass transfer channels, thereby improving catalytic performance for hydrogen evolution from ammonia borane hydrolysis (ABH). The turnover frequency of Ru/ONCB for ABH reaches 4529 ± 238 min −1 (determined based on Ru dispersion), surpassing a range of analogues and many previously reported carbon-supported Ru catalysts. This study presents a simple and rapid strategy to regulate the surface microenvironment of unfunctionalized carbon support, thereby enhancing the catalytic performance of its supported metal nanoparticles for catalytic hydrogen generation
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APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Jiaopeng Lai,Ruotao Zeng,Xinru Bian,Wen Leng,Cao Yang,Lihui Yang,Wei Li,Guangzhao Wang,Ganfeng He,Sihao Lv
Although the widely used dimensional stable anode (DSA) exhibits good activity and selectivity on chlorine evolution reaction (CER), the high content of precious metals and poor stability hinder the application. This work reported the use of interface engineering strategy to develop a cost-effective Ti 4 O 7 anode with ultralow Ru nanoparticles (NPs) loading (0.29 wt%) (Ru@Ti 4 O 7 ) via metal-support interactions. More oxygen vacancies were created by the interfacial Ru-O-Ti units and accelerated the reaction kinetics and charge transfer rate. 1 %Ru@Ti 4 O 7 displays superior CER activity, reaching a current density of 10 mA cm −2 at a low overpotential of 96.5 mV and a turnover frequency 16 times higher than DSA. The Ru@Ti 4 O 7 anode also achieved complete ammonia oxidation mainly mediated by chlorine radicals, with a high N 2 selectivity of 82 %. Particularly, the sustainable treatment for farm odor spray wastewater by the Ru@Ti 4 O 7 system was verified, in which the efficient purification of ammonia nitrogen and the good electrochemical stability of citric acid realized the recycling of water and deodorant. This work provides great opportunity to fabricate desirable Ti 4 O 7 –based CER electrodes and develops a good solution to the enormous challenges faced by the farm odor emission reduction industry.
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CHINESE JOURNAL OF CATALYSIS
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2024
·
IF 15.7
Tianhua Zhang,Haihui Hu,Jiaxin Li,Yinglong Gao,Lingling Li,Mingyuan Zhang,Xuanbei Peng,Yanliang Zhou,Jun Ni,Bingyu Lin,Jianxin Lin,Bing Zhu,Dongshuang Wu,Linjie Zhang,Lili Han,Lirong Zheng,Xiuyun Wang,Lilong Jiang
Ammonia (NH 3 ) is an excellent candidate for hydrogen storage and transport. However, producing NH 3 under mild conditions is a long-term, arduous task. Atomic cluster catalysts (ACCs) have been shown to be effective for catalytic N 2 -to-NH 3 conversion, opening the door to the development of efficient catalysts under mild conditions. Still, ACC formation with thermally stable catalytic sites remains a challenge because of their high surface free energy . Herein, we report anchoring Ba and/or Ce onto Ru ACCs (2 wt% Ru atomic clusters supported on N-doped carbon) to form so-called clusters–metal oxide promoters electronic interaction (CMEI) to stabilize the Ru atomic clusters. The resulting Ba/Ce/Ru ACCs significantly boost the NH 3 synthesis rate to 56.2 mmol NH3 g cat −1 h −1 at 400 °C and 1 MPa, which is 7.5-fold higher than that of Ru ACC. The strengthened CMEI between the Ba/Ce and Ru atomic clusters across the Ba/Ce/Ru ACC enables electron transfer from Ba and/or Ce to Ru atomic clusters. As such, the electron-enriched Ru atom could facilitate electron transfer to N≡N bond π* orbitals, which would weaken the N≡N bond and drive the eventual conversion of N 2 to NH 3 . This study offers insight into the role of CMEI in Ru ACCs and provides an effective approach for designing stable atomic cluster catalysts for NH 3 synthesis.
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MICROCHEMICAL JOURNAL
·
2025
·
IF 5.1
Xinyu Huang,Junhong Li,Huan Zhang,Xuemin Duan,Lihua Yao,Ruirui Yue,Jingkun Xu
As a natural flavonoid glycoside, rutin has been made into many medical products due to its unique pharmacological activity. However, excessive intake of rutin is harmful to health. Therefore, developing a new sensing technique to achieve highly sensitive, rapid and on-site detection of rutin is of great significance to ensure food and medicine safety. Herein, an electrochemical sensing platform was proposed based on the nanocomposite of functionalized multi-wall carbon nanotubes/poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate)/Ru nanoparticles (MWCNT-COOH/PEDOT:PSS/Ru) for rutin detection. The characterization techniques reveal that MWCNT-COOH and PEDOT:PSS crossed together forming a 3D interconnecting structure with plenty of areolations and high specific surface area, and Ru nanoparticles uniformly dispersed on the surface of MWCNT-COOH/PEDOT:PSS. Moreover, due to the good film reforming property of PEDOT:PSS, the as-obtained MWCNT-COOH/PEDOT:PSS/Ru composite shows special surface appearance as flexible free-standing film, which can be freely cut and used as sensing platform directly. Electrochemical experiments confirmed that MWCNT-COOH/PEDOT:PSS/Ru composite film performed satisfactory sensing properties toward rutin detection with wide linear ranges of 0.01 ∼ 0.7 μM and 0.7 ∼ 50 μM, low detection limit of 6.1 nM and high sensitivity of 79.43 μA μM −1 cm −2 . Besides, the composite sensing platform also exhibits high selectivity, reproducibility, and stability. During actual sample testing, the sensing platform was successfully applied for rutin detection in rutin pharmaceutical tablets and black buckwheat tea, showing promising application prospects in rapid, convenient, and high-efficiency on-site test.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Wenqin Zhao,Zonghao Zhang,Bo Wang,Yang Lv,Lei Huang,Pingle Liu
Catalytic hydrodeoxygenation is a plausible route to upgrade the quality of biomass energy sources. Herein, a series of Ru-Co alloy catalysts (Ru-Co/TiO 2 -Al 2 O 3 ) were prepared and applied in guaiacol hydrodeoxygenation to cyclohexanol. It was found that Ru-Co nanoparticles with average size of about 8.67 nm were uniformly dispersed on TiO 2 -Al 2 O 3 support. It was verified that Co doping led to the formation of electron-rich Ru and hence promoted the desorption of active hydrogen, while the constructed TiO 2 -Al 2 O 3 support possessed abundant oxygen vacancies and acidic sites, which facilitated adsorption and hydrogenolysis of −OCH 3 functional group. 5Ru-5Co/TiO 2 -Al 2 O 3 catalyst gives the best catalytic performance of >99% guaiacol conversion and 94% selectivity to cyclohexanol. In addition, the strong interactions between Ru-Co nanoparticles and TiO 2 -Al 2 O 3 could significantly inhibit aggregation and leaching of Ru-Co nanoparticles during the reaction. The research results will provide reference to design highly efficient and stable bimetallic catalysts in converting lignin-derived bio-oils.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Dexiang Zhang,Fujun Lan,Xiaomei Zhou,Yu Shu,Fu Li,Qingxin Guan,Mo Qiu,Wei Li
Amino acids are widely used in various applications, its production mainly relies on the fermentation of grain crops, and the chemosynthesis method from non-grain biomass still faces the challenge of low efficiency (<50 %). Herein, Ru clusters anchored on ultrathin TiO 2 nanobelts (NBs) with abundant oxygen vacancies are fabricated and used to convert lignocellulose-derived α-hydroxy acids to α-amino acids. The Ru/TiO 2 NBs achieved up to 80 % alanine yield from lignocellulose-derived lactic acid (LA). The characterization results reveal that the TiO 2 NBs with abundant oxygen vacancies could anchor Ru clusters uniformly and enable the α-OH dehydrogenation occur spontaneously. Simultaneously, Ru clusters with appropriate particle size are beneficial for the activation of H 2 and could promote the dehydrogenation from the α-OH and α-C(sp 3 )-H of LA. Furthermore, DFT simulations also indicate that further decrease the Ru cluster size (< 1 nm) will inhibit the adsorption of α-C(sp 3 )-H on cluster surface, thereby suppressing the removal of hydrogen atoms. This research provides a green and efficient chemical catalytic conversion idea for amino acid production from non-grain biomass.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Mingjing Ma,Huanhuan Yu,Baolin Zhu,Wenjun Zheng,Shoumin Zhang
The design of efficient catalysts with atom clusters (ACs) and single atoms (SAs) as active sites for water splitting presents an effective approach for improving bifunctional electrocatalytic performance by synergistically promoting electron transport and proton transfer kinetics. In this work, a series of Fe2O3-supported noble metal catalysts (M = Ru, Rh, Pd, Ag) incorporating both ACs and SAs sites were developed, with detailed characterization identifying Ru ACs as the primary active centers. The designed-interfacial M-O-Fe bonds play a critical role in charge redistribution, subsequently enhancing electron and proton transfer kinetics. The resulting heterostructure optimizes both the electronic environment and active site accessibility, yielding exceptional electrocatalytic performance. Further density functional theory calculations demonstrate that the incorporation of Ru species leads to increased filling of antibonding orbitals and modulation of the d-band center, subsequently reducing the energy barrier of the rate-determining steps to −0.267 eV for HER and 1.522 eV for OER, respectively. Consequently, the representative Ru/Fe2O3 with Ru content of 1.1 wt.% achieves an OER overpotential of 189 mV and a HER overpotential of 21 mV at a current density of 10 mA cm−2. This study highlights a novel approach to the design of advanced bifunctional electrocatalysts by engineering interfacial bridge bonds.
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