CHEMICAL ENGINEERING JOURNAL
·
2023
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IF 15.1
Hai Liu,Guoying Tan,Mengxuan Li,Zhuang Zhang,Marshet Getaye Sendeku,Yaping Li,Yun Kuang,Xiaoming Sun
Hydrogen evolution reaction is an important half-cell reaction in electrocatalytic water splitting process, which is an efficient way to store renewable energy into hydrogen fuel. However, grid scale water splitting always require high current densities up to amperes per square centimeter, which results change in local pH on the electrode surface, leading to instability risk of cathodic catalyst. Herein, a single atomic Ru doped WO 3 catalyst was fabricated, which exhibit excellent hydrogen evolution reaction (HER) activity with only 28.0, 17.6, and 83.0 mV in acidic, alkaline, and neutral media respectively as well as robust stability for 100 h at ampere-level current density is reported. Synchrotron radiation and density functional theory (DFT) calculations revealed that the defective oxygen and strong electron transfer from W sites to Ru not only achieved moderate H adsorption but also protected Ru sites from agglomeration, leading to superior HER activity and stability at industrial current density.
研究领域:
材料科学
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电化学
✓ 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
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催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
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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
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Science Bulletin
·
2023
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IF 18.9
Zhaolei Wang,Wenhai Xu,Guoying Tan,Xinxuan Duan,Bichen Yuan,Marshet Getaye Sendeku,Hai Liu,Tianshui Li,Fengmei Wang,Yun Kuang,Xiaoming Sun
Electrocatalytic two-electron water oxidation affords a promising approach for distributed production of H 2 O 2 using electricity. However, it suffers from the trade-off between the selectivity and high production rate of H 2 O 2 due to the lack of suitable electrocatalysts . In this study, single atoms of Ru were controllably introduced into titanium dioxide to produce H 2 O 2 through an electrocatalytic two-electron water oxidation reaction. The adsorption energy values of OH intermediates could be tuned by introducing Ru single atoms , offering superior H 2 O 2 production under high current density . Notably, a Faradaic efficiency of 62.8% with an H 2 O 2 production rate of 24.2 μmol min −1 cm −2 (>400 ppm within 10 min) was achieved at a current density of 120 mA cm −2 . Consequently, herein, the possibility of high-yield H 2 O 2 production under high current density was demonstrated and the importance of regulating intermediate adsorption during electrocatalysis was evidenced.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Kunjie Wang,Xianrong Liu,Yanan Li,Yunsi Wang,Riming Hu,Bingxin Liu,Peng Zhang,Benhua Xu,Yongcheng Li
Ensuring Ruthenium-based (Ru) catalysts with high metal utilization is a potential and challenging strategy for designing and constructing high catalytic activity electrocatalysts for hydrogen evolution reaction (HER). Herein, Ruthenium single atoms (SA) and Ruthenium nanoparticles (NPs) are simultaneously anchored on hierarchically porous carbon via the self-templates method for the first time. Benefiting from the synergetic effect of hierarchically porous carbon and the coexistence of Ru SA and Ru NPs, the Ru/C-800 shows attractive HER catalytic activity in acidic and alkaline solutions, with low overpotentials to drive the current density of 10 mA cm −2 and the smallest Tafel slope. Density functional theory (DFT) results reveal that the coexistence of Ru SA and Ru NPs can positively affect charge distribution and charge transfer kinetics, and reduce the hydrogen adsorption and water dissociation free energy. This work provides a novel self-templating strategy for synthesizing high catalytic activity catalysts in a wide pH range.
研究领域:
材料科学
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电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
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IF 21.1
Jinjing Qiu,Qi Chen,Cheng Liu,Yueling Chen,Jionghua Wu,Kaiqiang Jing,Jimmy C. Yu,Ling Wu,Xianzhi Fu
Defect engineering and single atom incorporation can provide more active sites to modulate the surface electronic structure of a catalyst and to activate reactant molecules. Herein, a series of Ru-anchored DUT-67(Zr) MOFs with explicit defect sites have been prepared for photocatalytic nitrogen reduction. It is characterized that Ru/DUT-67(Zr) possesses uniformly dispersed Ru single atoms and unsaturated Zr. Typically, 1.0 %Ru/DUT-67(Zr) shows best performance with a NH 4 + yield of 61.1 μmol·g −1 ·h −1 , which is approximately 6-folds higher than that of defective DUT-67(Zr) without Ru single atom (DUT-L), while pristine DUT-67(Zr) exhibits a lack of the photocatalytic N 2 reduction activity. The observed enhancement can be attributed to the introduction of Ru and unsaturated Zr sites induced by irradiation. Both of them can work together act as active centers to absorb and activate dinitrogen molecule. Furthermore, benefited from the electronic channel (Ru-S) between Ru and DUT-67(Zr), the separation of photogenerated carriers has been greatly improved, contributing to the collaborative conversion of activated N 2 to NH 3 . This study provides a new insight for designing a dual active sites photocatalyst with unsaturated coordinated sites and the single atoms by the coordinately interaction of functionalized linker.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2021
·Vol. 9
·期 20
·12196-12202
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IF 12.732
Yijun Li,Huijing Liu,Bing Li,Zhenzhen Yang,Zhenguo Guo,Jian-Bo He,Jianhui Xie,Tai-Chu Lau
Electrocatalytic water splitting is one of the most desirable ways to produce hydrogen, which is a clean and sustainable energy source. Improving the formation and the exposure of active sites is a key issue in the design of cost-effective and efficient metal-based electrocatalysts, especially for noble metals, in order to cut down the metal content and improve the mass activity of the metals, while maintaining high catalytic activity. Herein, we report a high-performance Ru-based electrocatalyst consisting of Ru single atoms and Ru nanoclusters encapsulated in highly porous N-doped carbon with abundant hierarchical pores (Ru/p-NC). Remarkably, Ru/p-NC shows excellent HER activity in 1.0 M KOH with a low overpotential of 10 mV at 10 mA cm−2, a small Tafel slope of 17 mV dec−1 as well as good durability for 24 h, outperforming commercial Pt/C and Ru/C catalysts. More importantly, the mass activity and turnover frequency (based on Ru loading) of Ru/p-NC are ultrahigh owing to the low loading of Ru, which are 17 A mgRu−1 and 8.9 H2 s−1, respectively, at a very low overpotential of 25 mV. Experimental results indicate that the porous N-doped carbon support not only leads to exposed active sites but also interacts strongly with the Ru moieties. In addition, it tunes the electronic structure of the catalyst, boosts the stability as well as facilitates mass transport and charge transfer kinetics. This work provides a new route for the synthesis of metal-based porous N-doped carbon hybrid electrocatalysts with abundant exposed active sites and strong metal-support interaction for energy conversion.
研究领域:
材料科学
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电化学
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能源转换
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Jiachen Li,Cong Zhang,Chi Zhang,Huijun Ma,Yong Yang,Zhaoqi Guo,Yaoyu Wang,Haixia Ma
Replacing sluggish oxygen evolution reaction (OER) by hydrazine oxidation reaction (HzOR) is an energy-saving approach to assist alkaline overall water splitting (OWS). However, it is still at the infant stage as the unsatisfactory of the design strategies for bifunctional catalysts toward both HzOR and hydrogen evolution, which leads to high working potential compared to the theoretical value. Here, for the first time, we report a galvanostatic immobilization of ruthenium single atoms (Ru SAs) into the oxygen vacancy of urchin-like tungsten trioxide (Vo-WO 3 ) and show low overpotentials of 17, 34, and 64 mV at –10 mA cm –2 under acid, alkaline, and neutral H 2 evolution, respectively. As an efficient bifunctional catalyst, the Vo-WO 3 /Ru SAs is firstly introduced to HzOR and achieves low working potential of –58 mV at 10 mA cm –2 . The HzOR-assisted OWS also delivers an ultralow cell voltage of only 25 mV at 10 mA cm –2 in alkaline medium, which is far beyond the platinum and most of the state-of-the-art catalysts. Additionally, this coupled system can also be well performed under neutral condition, realizing a cell voltage of only 137 mV at 10 mA cm –2 . The excellent pH-universal HzOR-assisted OWS activity is attributed to the particular electronic configuration between Ru SAs and WO 3 , the immobilization of Ru SAs in WO 3 could induce electron redistribution and optimize free energy of hydrogen adsorption in hydrogen evolution, while the isolation of Ru SAs also leads to the electropositivity of W sites and tends to accelerate the oxidation of hydrazine.
研究领域:
材料科学
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催化化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry C
·
2023
·Vol. 11
·期 19
·6336-6346
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IF 6.4
Dong Guo,Chen Chen,Yongqiang Wang,Youke Wang,Conglu Zhang
Two dimensional materials show unique advantages in catalysis. In this work, it was found that melamine could induce the directional growth of cobalt-based catalysts to form an ultra-thin two-dimensional hexagonal nanosheet structure with only 1.5 nm. In addition, these hexagonal nanosheets (HNs) could grow into a microporous structure under high temperature conditions, and the finally formed CoO hexagonal porous nanosheets (HPNs) had a surface area 11.3 times that of the nanoparticles. Embedding 1.25 wt% of monoatomic ruthenium in the CoO HPNs (CoO/Ru1.25% HPNs) allowed the catalyst to have more active charge storage and transfer centers. The results showed that the overpotential of CoO/Ru1.25% HPNs was 64 mV lower than that of CoO nanoparticles at 10 mA cm−2. The Tafel slope of CoO/Ru1.25% HPNs was only half that of CoO nanoparticles, indicating that a small amount of Ru dispersion and the two-dimensional structure control significantly increased the kinetic rate in the oxygen evolution reaction. The DFT results showed that the Ru single atoms in CoO/Ru HPNs (111) possessed the lowest energy barrier (1.19 eV). The Ru single atoms could effectively reconstruct the neighboring localized structure in the formation of ˙OOH, which desirably decreased the free energy of the system.
研究领域:
催化材料
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能源化学
·
理论计算
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2024
·Vol. 15
·期 1
·1-13
·
IF 14.7
Jia Hongnan,Yao Na,Jin Yiming,Wu Liqing,Zhu Juan,Luo Wei
Suppressing the kinetically favorable lattice oxygen oxidation mechanism pathway and triggering the adsorbate evolution mechanism pathway at the expense of activity are the state-of-the-art strategies for Ru-based electrocatalysts toward acidic water oxidation. Herein, atomically dispersed Ru species are anchored into an acidic stable vinyl-linked 2D covalent organic framework with unique crossed π-conjugation, termed as COF-205-Ru. The crossed π-conjugated structure of COF-205-Ru not only suppresses the dissolution of Ru through strong Ru-N motifs, but also reduces the oxidation state of Ru by multiple π-conjugations, thereby activating the oxygen coordinated to Ru and stabilizing the oxygen vacancies during oxygen evolution process. Experimental results including X-ray absorption spectroscopy, in situ Raman spectroscopy, in situ powder X-ray diffraction patterns, and theoretical calculations unveil the activated oxygen with elevated energy level of O 2 p band, decreased oxygen vacancy formation energy, promoted electrochemical stability, and significantly reduced energy barrier of potential determining step for acidic water oxidation. Consequently, the obtained COF-205-Ru displays a high mass activity with 2659.3 A g −1 , which is 32-fold higher than the commercial RuO 2 , and retains long-term durability of over 280 h. This work provides a strategy to simultaneously promote the stability and activity of Ru-based catalysts for acidic water oxidation.
研究领域:
材料科学
·
电化学
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催化反应
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Catalysis
·
2020
·
IF 12.35
Xiuyun Wang,Lingling Li,Zhongpu Fang,Yongfan Zhang,Jun Ni,Bingyu Lin,Lirong Zheng,Chak-tong Au,Lilong Jiang
The industrial synthesis of NH3 using Fe- or Ru-based catalysts usually requires harsh reaction conditions. It is desirable to develop catalysts that perform well at low temperature and pressure (250–400 °C, <2 MPa). The main challenge of low-temperature NH3 synthesis is the dissociation of the extremely stable N≡N triple bond. Herein, we report the design of homogeneous single-atom Ru centers on an H-ZMS-5 (HZ) support with the Ru atoms individually anchored in the micropores of HZ, effectively boosting NH3 synthesis under mild conditions via an associative pathway. Synchrotron-based near-edge X-ray absorption fine structure (NEXAFS) and in situ DRIFTS analyses show that ═N– groups are the primary intermediates, and DFT calculations further show that, unlike Ru nanoclusters, the cooperation of a single Ru atom and hydrogen species in HZ leads to N2 hydrogenation rather than direct N2 dissociation, and the indirect N–N bond dissociation occurs much more easily via the formation of the NHNH3* intermediate; the energy barrier for breaking the N–N bond keeps falling from 2.90 eV for *N2 to 0.04 eV for *NHNH3, showing that N2 hydrogenation is an effective way for sharp weakening of N–N bonds. Moreover, the rate-determining step is shifted from the dissociation of the N≡N triple bond to the formation of *N2H2. As a consequence, the single-atom 0.2 wt % Ru/H-ZSM-5 catalyst shows the highest NH3 synthesis rate per gram of Ru (1.26 molNH3 gRu–1 h–1 at 300 °C and 1 MPa) among the Ru-based catalysts ever reported.
研究领域:
催化化学
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材料科学
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理论计算化学
✓ 已验证
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2021
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IF 6.986
Xiaoli Xie,Dong Ping Wang,Chunxian Guo,Yuhang Liu,Qianghai Rao,Fangming Lou,Qiannan Li,Yongqiang Dong,Qunfang Li,Hong Bin Yang,Fang Xin Hu
Single-atom catalysts have attracted numerous attention due to the high utilization of metallic atoms, abundant active sites, and highly catalytic activities. Herein, a single-atom ruthenium biomimetic enzyme (Ru-Ala-C3N4) is prepared by dispersing Ru atoms on a carbon nitride support for the simultaneous electrochemical detection of dopamine (DA) and uric acid (UA), which are coexisting important biological molecules involving in many physiological and pathological aspects. The morphology and elemental states of the single-atom Ru catalyst are studied by transmission electron microscopy, energy dispersive X-ray elemental mapping, high-angle annular dark field–scanning transmission electron microscopy, and high-resolution X-ray photoelectron spectroscopy. Results show that Ru atoms atomically disperse throughout the C3N4 support by Ru–N chemical bonds. The electrochemical characterizations indicate that the Ru-Ala-C3N4 biosensor can simultaneously detect the oxidation of DA and UA with a separation of peak potential of 180 mV with high sensitivity and excellent selectivity. The calibration curves for DA and UA range from 0.06 to 490 and 0.5 to 2135 μM with detection limits of 20 and 170 nM, respectively. Moreover, the biosensor was applied to detect DA and UA in real biological serum samples using the standard addition method with satisfactory results.
研究领域:
生物医学工程
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材料科学
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分析化学
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）