JOURNAL OF ELECTROANALYTICAL CHEMISTRY
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2021
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IF 4.464
Fuad Abduro Bushira,Shimeles Addisu Kitte,Haijuan Li,Lirong Zheng,Ping Wang,Yongdong Jin
Simultaneous highly sensitive and accurate detection of dopamine (DA) and uric acid (UA) is of great importance since they are important biomolecules that are commonly coexisted in the human body and play a crucial role in numerous physiological and pathological features. In this work, Fe-N 5 single atom catalyst (SAC) supported on graphene was firstly employed for simultaneous electrochemical detection DA and UA. Owing to its unique electronic structure and abundant active sites, under optimal conditions, the enzyme-like Fe-N 5 SAC constructed electrochemical (bio)sensor exhibits excellent linear characteristic responses in the range of 0.005–500 and 0.01–480 µM, as well as the low limit of detection of 0.007 and 0.027 nM for DA and UA, respectively. More critically, the developed electrochemical system shows promising merits of exceptional stability, good repeatability, and, consequently, it was successfully applied for simultaneous sensitive detection of DA and UA in human serum samples.
研究领域:
生物医学工程
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分析化学
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DOI
高影响因子
Materials
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2024
·Vol. 17
·期 13
·3058
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IF 3.1
Ziyue Wang,Ying Zhang,Hao Zhang,Qingdi Sun,Xiaohui He,Hongbing Ji
As worldwide plastic pollution continues to rise, innovative ideas for effective reuse and recycling of waste plastic are needed. Single-atom catalysts (SACs), which are known for their high activity and selectivity, present unique advantages in facilitating plastic degradation and conversion. Waste plastic can be used as a support or raw material to create SACs, which reduces waste generation while simultaneously utilizing waste as a resource. This work successfully utilized waste plastic polyurethane (PU) as a support, through a unique Rapid Thermal Processing Reactor (RTPR) to synthesize an efficient Pd1/PU SACs. At 25 °C and 0.5 MPa H2, Pd1/PU displayed outstanding activity and selectivity in the hydrogenation of styrene, as well as remarkable stability. Pd1/PU performed well in hydrogenating a variety of common substrates. These findings highlight the great potential of SACs in plastic waste reuse and recycling, offering intriguing solutions to the global plastic pollution problem.
研究领域:
环境科学
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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
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2024
·
IF 18.8
Yida Zhang,Zhentao Ma,Shaokang Yang,Qingyu Wang,Limin Liu,Yu Bai,Dewei Rao,Gongming Wang,Hongliang Li,Xusheng Zheng
Catalytic conversion of nitrate (NO 3 − ) pollutants into ammonia (NH 3 ) offers a sustainable and promising route for both wastewater treatment and NH 3 synthesis. Alkali cations are prevalent in nitrate solutions, but their roles beyond charge balance in catalytic NO 3 − conversion have been generally ignored. Herein, we report the promotion effect of K + cations in KNO 3 solution for NO 3 − reduction over a TiO 2 -supported Ni single-atom catalyst (Ni 1 /TiO 2 ). For photocatalytic NO 3 − reduction reaction, Ni 1 /TiO 2 exhibited a 1.9-fold NH 3 yield rate with nearly 100% selectivity in KNO 3 solution relative to that in NaNO 3 solution. Mechanistic studies reveal that the K + cations from KNO 3 gradually bonded with the surface of Ni 1 /TiO 2 , in situ forming a K-O-Ni moiety during reaction, whereas the Na + ions were unable to interact with the catalyst in NaNO 3 solution. The charge accumulation on the Ni sites induced by the incorporation of K atom promoted the adsorption and activation of NO 3 − . Furthermore, the K-O-Ni moiety facilitated the multiple proton-electron coupling of NO 3 − into NH 3 by stabilizing the intermediates.
研究领域:
环境科学
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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
ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2024
·
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
CHINESE JOURNAL OF CATALYSIS
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2024
·
IF 15.7
Qian Zhang,Xunzhu Jiang,Yang Su,Yang Zhao,Botao Qiao
With the increasing production of propane from shale gas and the growing demand for propylene, propane dehydrogenation (PDH) has gained significant attention as a promising route for the on-purpose production of propylene. As a cheap yet efficient catalyst, Ni-based catalysts have attracted interest because of its ability to activate alkane. Single-atom catalysts (SACs) can maximize the metal atom utilization. Here, we demonstrate that anatase TiO 2 supported Ni SAC (Ni 1 /A-TiO 2 ) exhibits not only superior intrinsic activity and propylene selectivity but also much better stability than the corresponding Ni nanoparticle (NP) catalyst (Ni NP /A-TiO 2 ) in PDH reaction at 580 °C. The rate of propylene production on Ni 1 /A-TiO 2 is about 1.96 mol C3H6 g Ni −1 h −1 , about 65 times higher than that of Ni NP /A-TiO 2 sample (0.03 mol C3H6 g Ni −1 h −1 ). In combination of high-angle annular dark-field scanning transmission electron microscopy, in-situ diffuse reflectance infrared Fourier transform spectra, in-situ X-ray photoelectron spectroscopy and X-ray absorption spectroscopy characterizations, we confirm that the Ni SAC mainly contains individual Ni atom singly dispersed on the support in positive Ni (II) valence state. In addition, as a result of strong metal-support interaction (SMSI) between Ni NP and TiO 2 carrier under reduced conditions, the Ni NPs sites are encapsulated by TiO x overlayer (~2 nm thick) thus display poor reaction performance.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Fang Dong,Yu Meng,Weitong Ling,Weigao Han,Weiliang Han,Xiaona Li,Zhicheng Tang
Development of low-cost noble Pt-based catalyst with superior catalytic performance is a challenge to achieve its application in VOCs catalytic oxidation. Although the single atom provides a strategy to design and develop highly efficient heterogeneous catalysts that simultaneously maximizes the utilization of precious metal atoms, the stability of single atom catalysts is not satisfactory as a result of its high atomic surface energy. Here we construct a Pt 1 @CeO 2 single atom catalyst (SAC) with excellent catalytic activity for benzene catalytic combustion (T 90 = 212 °C) and low precious metal Pt loading, and even displaying an outstanding thermal stability and water resistance under the harsh conditions of 30,000 mL/g/h and 2000 ppm benzene. This Pt 1 @CeO 2 catalyst was obtained by in situ domain limited encapsulation of Pt species in Ce-MOFs nanocages during the solvothermal reaction process. It is observed that lots of oxygen vacancies were created by the dislocation and phase transition of CeO 2 to provide abundant sites for anchoring single atomic Pt, which can be localized and anchored firmly to oxygen vacancies, thus forming the highly stable Pt single atom. The atomically dispersed Pt is capable of improving the catalytic activity by forming Pt-O band. The good water resistance may be ascribed to the confined Pt single atom into oxygen vacancies of CeO 2 support to form strong metal-support interaction (SMSI), and the PtO x nanoparticles would be easy to aggregate deactivation under water vapor conditions. It is a simple and universal strategy to prepare Pt SAC via the inherently confined space of MOFs nanocages formed by coordination of organic ligands and metal ions, which benefits from the functional modification of ethylene glycol in MOFs self-assembly reaction.
研究领域:
材料科学
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环境科学
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产品关联
DOI
高影响因子
ChemSusChem
·
2024
·
IF 7.5
Yixian Liu,Mengling Zhang,Kaili Bao,Hui Huang,Zhenhui Kang
Graphical The catalyst comprised of Cu single atoms loaded on carbon substrate is developed for highly selective electrocatalytic reduction of CO 2 to CH 4 , which exhibits over 50 % FE for CH 4 within a wide potential window. Electrocatalytic carbon dioxide reduction into high-value chemicals is one of the important solutions to the greenhouse effect and energy crisis. However, the slow kinetic process of eight electrons requires the development of efficient catalysts to improve the yields. Single atom catalysts (SACs) with high activity and selectivity have become an emerging research frontier in the field of heterogeneous catalysis. Herein, a catalyst comprised of Cu single atoms loaded on carbon substrate (Cu-NC) is developed for highly selective electrocatalytic reduction of CO 2 to methane (CH 4 ). The optimal catalyst (Cu-NC-1-4) exhibits a faradaic efficiency (FE) of over 50 % for CH 4 within a wide potential window from −1.3 V to −1.8 V ( vs . RHE) and the highest FE of CH 4 is up to 67.22 % at −1.6 V ( vs . RHE). Meanwhile, the product selectivity of CH 4 among all the carbon products reaches 93.00 %, and the activity decay can be negligible via the 70-hour-stability-test. The existence of atomic dispersed Cu−N 3 sites was verified by high-angle annular dark field scanning transmission electron microscopy (HAADF-STEM) and X-ray absorption near edge structure (XANES). Density functional theory (DFT) calculations show that the effective adsorption of the key intermediate *CO on Cu−N 3 sites prompts the generation of CH 4 .
研究领域:
化学
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nano Research
·
2024
·
IF 9.5
Israr Muhammad,Humayun Muhammad,Zhang Jiaqi,Shah Khadim,Tan Xin,Chen Chen,Li Yadong
To address the sluggish kinetics of the oxygen evolution reaction (OER), a potential approach is to rationally design and fabricate extremely effective single atom catalysts (SACs). Using an appropriate matrix to stabilize single-atom active centers with optimal geometric and electronic structures is crucial for enhancing catalytic activity. Herein, we report the design and fabrication of Ir single atoms on NiFeZn layered double hydroxide (Ir-SAC/NiFeZn-LDH) electrocatalyst for highly efficient and stable OER. It is investigated that the NiFeZn support exhibits abundant defect sites and unsaturated coordination sites. These sites function to anchor and stabilize single Ir single atoms on the support. The strong synergetic electronic interaction between the Ir single atoms and the NiFeZn matrix resulted in remarkable OER performance of the as-fabricated Ir-SAC/NiFeZn catalyst. With a loading Ir content of 1.09 wt.%, this catalyst demonstrates a highly stable OER activity, with an overpotential of 196 mV at 10 mA·cm −2 and a small Tafel slope of 35 mV·dec −1 for the OER in a 1 M KOH solution. These results significantly surpass the performance of the commercially available IrO 2 catalyst.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Lijin Gan,Zekun Liu,Lei Feng,Yi Duan,Guangyuan Xu,Si Chen,Huan Yan
Adipic aldehyde, a precursor for polymers, has significant industrial applications, where the hydroformylation of 1,3-butadiene is a promising route to fabricate adipic aldehyde. However, the heterogeneous hydroformylation of 1,3-butadiene has been rarely reported. In this work, we reported ligand-modified Rh-supported single-atom catalysts and investigated them for efficient hydroformylation of 1,3-butadiene. Among the selected phosphine ligand candidates, the L11 ligand (NiXantphos) coordinated Rh atoms could achieve the highest selectivity to adipic aldehyde. Furthermore, in situ CO DRIFTS indicated that active species similar to homogeneous catalysts were formed on the surface of the ligand modified and supported Rh catalyst during the reaction, demonstrating the similar hydroformylation mechanism and origins of the various products.
研究领域:
催化化学
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工业化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Zhiqiang Wang,Xiaomei Zhou,Gehui Wang,Qing Tong,Haiqin Wan,Lin Dong
The elimination of toluene is an obligatory target with increasing VOC emission in recent years. This study successfully prepared a single-atom Ir catalyst (Ir1/CeO2) by a simple incipient wetness impregnation method, confirmed by in situ CO DRIFTS and AC-HAADF-STEM. Compared to the cluster Ir catalyst (Ir/CeO2-C), Ir1/CeO2 exhibited excellent catalytic performance, stability, and water resistance for the oxidation of toluene. By Raman, H2-TPR, O2-TPD, and XPS experiments, abundant oxygen defects and a unique Ir3+–Ov–Ce3+ structure were formed for the Ir1/CeO2 sample because it had a lower oxygen vacancy formation energy. Furthermore, the DFT results revealed that the Ir1/CeO2 sample had a lower ring-opening energy barrier and adsorption energy of the ring-opening products, which was the rate-determining step for the oxidation of toluene. This work provides instructive insights into the construction of Ir/CeO2 catalysts for the highly efficient removal of VOCs.
研究领域:
催化化学
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JACS Au
·
2024
·
IF 8.5
Xixi Liu,Liang Huang,Yurong He,Peng Zhou,Xuedan Song,Zehui Zhang
It remains challenging to construct C═N bonds due to their facile hydrogenation. Herein, a single Co atom catalyst was discovered to be active for the selective construction of C═N bonds toward the synthesis of imines and N-heterocycles via reductive coupling of nitroarenes with various alcohols, including inert aliphatic ones. DFT calculations and experimental data revealed that the transfer hydrogenation proceeded via the intramolecular hydride transfer and the transfer of H from the α-Csp3-H bond to the nitro group was the rate-determining step. The single Co atoms served as a bridge to transfer the electrons from the catalyst to the adsorbed alcohol molecules, resulting in the activation of the α-Csp3-H bond. Unlike metal nanoparticles, the C═N bonds in imine products can be reserved due to the large steric hindrance from substituents on C and N. DFT calculation also confirmed that transfer hydrogenation of the C═N bonds in imines is thermodynamically unfavored with a much higher energy barrier compared with the transfer hydrogenation of the –NO2 group (1.47 vs 1.15 eV).
研究领域:
化学
·
催化反应
·
理论计算
✓ 已验证
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
·
2020
·
IF 6.785
Pei-Hua Li,Meng Yang,Yi-Xiang Li,Zong-Yin Song,Jin-Huai Liu,Chu-Hong Lin,Jie Zeng,Xing-Jiu Huang
Achieving highly sensitive and selective detection of trace-level As(III) and clarifying the underlying mechanism is still a intractable problem. The electroanalysis of As(III) relies on the electrocatalytic ability of the sensing interface. Herein, we first adopt single-atom catalysts as the electrocatalyst in As(III) detection. Cobalt single-atoms anchored on nitrogen-doped carbon material (Co SAC) were found to have an extraordinary sensitivity of 11.44 μA ppb–1 with excellent stability and repeatability, which so far is the highest among non-noble metal nanomaterials. Co SAC also exhibited a superior selectivity toward As(III) compared with some bivalent heavy metal ions (HMIs). Combining X-ray absorption spectroscopy (XAFS), density functional theory (DFT) calculation, and reaction kinetics simulation, we demonstrated that Co single atoms stabilized in N2C2 support serve as active sites to catalyze H3AsO3 reduction via the formation of Co–O hybridization bond, leading to a lower energy barrier, promoting the breakage of As–O bonds. Importantly, the first electron transfer is the rate-limiting step of arsenic reduction and is found to be more favorable on Co-SAC both thermodynamically and kinetically. This work not only expands the potential applicaiton of single-atom catalysts in the detection and treatment of As(III), but also provides atomic-level catalytic insights into HMIs sensing interfaces.
研究领域:
环境科学
·
材料科学
·
分析化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）