ACS Catalysis
·
2022
·
IF 13.7
Biao Hu,Bing-Hao Wang,Lang Chen,Zhang-Jun Bai,Wei Zhou,Jun-Kang Guo,Sheng Shen,Ting-Liang Xie,Chak-Tong Au,Li-Long Jiang,Shuang-Feng Yin
In the design of photocatalysts for ammonia synthesis, the construction of effective nitrogen (N2) adsorption and activation sites is critical. Herein, Fe single atoms were effectively fixed on the surfaces of WO2.72–x nanowires. Electronic interactions between single Fe atoms and WO2.72–x resulted in a d-band center shift toward the Fermi level and thus enhancement of N2 bonding with the catalyst surface. The studies of differential charge density and electron localization reveal that there is enhanced electron transfer from Fe-SA/WO2.72–x to the adsorbed N2, signifying that Fe single atoms are active centers for N2 activation. Benefiting from electronic interactions, the optimized catalyst shows a NH4+ generation rate of 186.5 μmol g–1 h–1 during photocatalytic N2 reduction.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
CARBON
·
2024
·
IF 10.5
Ying Su,Bin Jiang,Haochen Shen,Na Yang,Xiaowei Tantai,Xiaoming Xiao,Yongli Sun,Luhong Zhang
Carbon materials have obtained some achievements in electromagnetic wave (EMW) absorption owing to their excellent electrical conductivity and low density. However, poor impedance matching and high electrical conductivity limit their EMW absorption properties. Metal single atoms absorbers have garnered considerable attention in EMW absorption, largely due to the high metal availability and special coordination structure, but the modulation of the EMW absorption properties still needs to be improved. Herein, atomically dispersed Fe sites embedded into the N-doped mesoporous carbon spheres (Fe–SAs/NC) were synthesized through a facile coordination-assisted polymerization assembly strategy without acid leaching treatment. Benefitting from abundant mesoporous structure, the Fe–SAs/NC displays large specific surface area (339 m 2 g −1 ) and optimized impedance matching, which results in an effective reduction of the absorber density. The homogeneously dispersed Fe single atoms (Fe–SAs) on the carbon skeleton lead to the improvement in conduction and dipole polarization losses of Fe–SAs/NC, which endows Fe–SAs/NC with exceptional EMW absorption properties. Experimental results indicate that Fe–SAs/NC displays desirable EMW absorption properties with the minimal reflection loss of −52.5 dB at 2.8 mm and the effective absorption bandwidth of 4.8 GHz. The study provides valuable insights for the development of carbon materials modified with atomically dispersed metal sites to achieve high-efficient EMW absorbers.
研究领域:
材料科学
·
电磁学
·
纳米技术
✓ 已验证
DOI
高影响因子
Chem Catalysis
·
2024
·
IF 11.5
Lei Wang,Panjie Guo,Yun Han,Chao Han,Hai Sun,Run Huang,Xuan Liu,Mengting Huang,Zhelin Mao,Xuecheng Yan,Aijun Du,Xin Wang
Electrocatalytic nitrate reduction to ammonia (NO 3 RR) opens a feasible approach to both wastewater treatment and ammonia production. However, the key catalyst materials still suffer from low activity, especially in neutral medium. Here we report that a tandem catalyst obtained by coupling atomic Fe sites (Fe SA ) with Fe nanoparticles (Fe NP ) in carbon supports high-performance NO 3 RR. It can deliver a maximum NH 3 faradaic efficiency of 95.5% at −0.85 V and a high NH 3 yield rate of 4042 μg h −1 mg cat −1 at −0.9 V, ranked among the top-performing catalysts reported. The combined experimental and theoretical analyses demonstrate the synergistic effect for dual sites consisting of Fe SA and corresponding Fe NP , as well as the tandem-enhanced NO 3 RR mechanism whereby Fe SA spontaneously adsorbs and activates NO 3 to form ∗NO intermediates while Fe NP accelerates water dissociation to provide more ∗H, thus promoting the following hydrogenation process and leading to consequent tandem-enhanced NO 3 RR activity.
研究领域:
电化学
·
催化材料
·
环境科学
·
能源化工
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Ruirui Yun,Feiyang Zhan,Na Li,Beibei Zhang,Wanjiao Ma,Lirui Hong,Tian Sheng,Liting Du,Baishu Zheng,Shoujie Liu
In the area of catalysis, selective reduction of nitro compounds to amino compounds is a colossal challenge due to the existence of competitive reducible functional groups. Herein, an Fe-based catalyst FeSAs/Fe2O3ACs/N-doped polyhedral carbon (NPC) has been designed and synthesized. As we expected, compared with FeSAs and FeNPs, FeSAs/Fe2O3ACs/NPC shows excellent catalytic performance (turnover frequency up to 1923 h–1, calculated with nitrobenzene), chemoselectivity, and tolerance during the hydrogenation reaction of nitro compounds under room temperature because of the synergistic effects between FeSAs and Fe2O3ACs. The theoretical calculations show that FeSAs prefers to undergo hydrazine decomposition to generate hydrogen and the Fe2O3ACs surface is more active toward the nitrobenzene reduction to aniline.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Guohao Zhu,Ze Li,Hao Guo,Guangchao Li,Youbin Zheng,Xin Liu,Haijun Pan,Liang Dong,Jianbing Zang,Shaopei Jia
Despite having a similar electronic structure to Pt, TiN exhibits poor catalytic activity for oxygen reduction reaction (ORR). Doping transition metal (M) atoms into TiN can enhance its ORR catalytic activity by creating MN x structures similar to those found in M and N codoped carbon materials . Notably, TiN demonstrates better stability than carbon materials. Herein, a hybrid of M-doped TiN and N-doped carbon nanofibers (M-TiN/NCNFs) was prepared via electrospinning followed by thermal treatment. Among the prepared M-TiN/NCNFs, Fe-TiN/NCNFs exhibited the highest ORR catalytic activity and excellent stability. The FeN 5 structure in Fe-TiN/NCNFs was identified as the active site. Density functional theory calculations indicated the moderate interaction between Fe and O (Fe–O bond) is a key factor for the optimal ORR catalytic activity of Fe-TiN/NCNFs. The number of antibonding electrons in molecular orbital of M–O bond can serve as a descriptor for distinguishing the ORR catalytic activities of M-TiN/NCNFs.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
Cell Reports Physical Science
·
2022
·
IF 7.832
Xiao Wang,Lei Sun,Wei Zhou,Li Yang,Guoqing Ren,Hao Wu,Wei-Qiao Deng
The exploration of environmentally friendly and highly efficient oxygen evolution reaction (OER) catalysts is vital to large-scale, electrochemical renewable-fuels generation. Here, we report an iron single-atom catalyst (SAC) confined in a covalent organic framework (Fe-SAC@COF), which constitutes an unusual Fe–NO coordination in the skeleton. The as-prepared Fe-SAC@COF exhibits a high mass activity of 9.20 A mg −1 , which is 1.95 times higher than Ni species of the same coordination and 5.05 times higher than nanoparticulate Fe counterpart. Moreover, it shows, to the best of our knowledge, a record-low overpotential (290 mV) and Tafel slope (40 mV dec −1 ) among the reported atomically dispersed Fe-based catalysts and surpasses the benchmark Ir/C catalyst. The density functional theory calculation shows that the Fe–NO coordination exhibits low binding energy of oxygenated intermediates, which leads to an outstanding electrocatalytic OER performance. This work provides design strategies toward unusually coordinated SACs by prudent COF confinement for advanced electrocatalysis.
研究领域:
材料科学
·
电化学
·
催化科学
✓ 已验证
DOI
高影响因子
Nanomaterials
·
2022
·Vol. 12
·期 9
·1593
·
IF 5.719
Yining Jia,Chunjing Shi,Wei Zhang,Wei Xia,Ming Hu,Rong Huang,Ruijuan Qi
Single-atom non-precious metal oxygen reduction reaction (ORR) catalysts have attracted much attention due to their low cost, high selectivity, and high activity. Herein, we successfully prepared iron single atoms anchored on nitrogen-doped carbon matrix/nanotube hybrid supports (FeSA-NC/CNTs) by the pyrolysis of Fe-doped zeolitic imidazolate frameworks. The nitrogen-doped carbon matrix/carbon nanotube hybrid supports exhibit a specific surface area of 1626.814 m2g−1, which may facilitate electron transfer and oxygen mass transport within the catalyst and be beneficial to ORR performance. Further electrochemical results revealed that our FeSA-NC/CNTs catalyst exhibited excellent ORR activity (half-wave potential: 0.86 V; kinetic current density: 39.3 mA cm−2at 0.8 V), superior to that of commercial Pt/C catalyst (half-wave potential: 0.846 V; kinetic current density: 14.4 mA cm−2at 0.8 V). It also has a great stability, which makes it possible to be a valuable non-noble metal electrode material that may replace the latest commercial Pt/C catalyst in the future.
研究领域:
材料科学
·
电化学
✓ 已验证
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Xin Mao,Zhaoyan Deng,Yiming Liu,Haiyang Xie,Qian He,Yanjuan Zhang,Zuqiang Huang,Huayu Hu,Tao Gan
Ultra-small metal clusters have emerged as one of the most promising alternatives to heterogeneous Fenton-like catalysts. Despite the high atom utilization and structural stability of catalysts with ultra-small clusters and single-atom sites, there is still challenging for the synthesis of these catalysts due to their facile aggregation. Herein, we successfully fabricated a catalyst (Fe-NC-900) with single-atom sites and ultra-small clusters by a ball milling method combined with subsequent pyrolysis process. Fe-NC-900 showed high efficiency and superior stability in the activation of peroxymonosulfate (PMS) for catalytic oxidation of refractory organic compounds. Chemical quenching experiments, electron paramagnetic resonance (EPR), in-situ Raman spectra, and electrochemical analysis indicated that the 1 O 2 oxidation was the main non-radical pathway rather than the high-valent iron oxidation and electron transfer mechanism for the degradation of RhB in the Fe-NC-900/PMS system. This work provides useful insights into the design and synthesis of the catalysts with single atoms and ultra-small clusters for practical applications in Fenton-like catalytic processes.
研究领域:
环境催化
·
材料化学
·
纳米环境技术
·
高级氧化过程
·
污染物降解
✓ 已验证
DOI
高影响因子
Nano Research
·
2024
·
IF 9.5
Sun Yudie,Han Yunxiang,Wang Mingyue,Ye Mingfu,Wu Konglin,Zhang Kui
Circulating microRNAs (miRNAs) play a pivotal role in the occurrence and development of acute myocardial infarction (AMI), and precise detection of them holds significant clinical implications. The development of luminol-based luminophores in the field of electrochemiluminescence (ECL) for miRNA detection has been significant, while their effectiveness is hindered by the instability of co-reactant hydrogen peroxide (H 2 O 2 ). In this work, an iron single-atom catalyst (Fe-PNC) was employed for catalyzing the luminol-O 2 ECL system to achieve ultra-sensitive detection of myocardial miRNA. Target miRNA triggers a hybridization chain reaction (HCR), resulting in the generation of a DNA product featuring multiple sticky ends that facilitate the attachment of Fe-PNC probes to the electrode surface. The Fe-PNC catalyst exhibits high promise and efficiency for the oxygen reduction reaction (ORR) in electrochemical energy conversion systems. The resulting ECL biosensor allowed ultrasensitive detection of myocardial miRNA with a low detection limit of 0.42 fM and a wide linear range from 1 fM to 1.0 nM. Additionally, it demonstrates exceptional performance when evaluated using serum samples collected from patients with AMI. This work expands the application of single-atom catalysis in ECL sensing and introduces novel perspectives for utilizing ECL in disease diagnosis.
研究领域:
生物传感器
·
电化学
·
纳米技术
·
心脏病学
·
分子诊断
✓ 已验证
DOI
高影响因子
Nano Research
·
2024
·Vol. 17
·期 6
·4924-4933
·
IF 9.5
Fan Yu,Yi Yu,Rong Hongpan,Zhang Jiatao
Carbon-based single-atom catalysts (SACs) have been widely studied in the field of biomedicine due to their excellent catalytic performance. However, carbon-based SACs usually aggregate during pyrolysis, which leads to the reduction of catalytic activity. Here, we describe a method to improve the monodispersion of SACs using silicon dioxide as a protective layer. The decoration of silicon dioxide serves as a buffer layer for individual nanoparticles, which is not destroyed during the pyrolysis process, ensuring the single-particle dispersion of the nanoparticles after etching. This approach increased the hydroxyl groups on the surface of Fe-SAC (Fe-SAC-SE) and improved its water solubility, resulting in a four times enhancement of the peroxidase (POD)-like activity of Fe-SAC-SE (58.4 U/mg) than that of non-protected SACs (13.9 U/mg). The SiO 2 -protection approach could also improve the catalytic activities of SACs with other metals such as Mn, Co, Ni, and Cu, indicating its generality for SACs preparation. Taking advantage of the high POD-like activity, photothermal properties, and large specific surface area of Fe-SAC-SE, we constructed a synergistic therapeutic system (Fe-SAC-SE@DOX@PEG) for combining the photothermal therapy, catalytic therapy, and chemotherapy. It was verified that the photothermal properties of Fe-SAC-SE@DOX@PEG could effectively improve its POD-like activity, exhibiting excellent tumor-killing performance at the cellular level. This work may provide a general approach to improve the performances of SACs for disease therapy and diagnosis.
研究领域:
生物医学工程
·
纳米技术
·
催化
·
材料科学
·
肿瘤学
·
诊疗学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Xinyi Li,Jingjing Liu,Qinghai Cai,Ziwang Kan,Song Liu,Jingxiang Zhao
Modulating the microenvironment of single-metal active sites holds excellent promises for developing highly efficiently oxygen electrocatalysts. Herein, by combining theoretical predictions and experiments, we reported a general strategy to engineer the electronic properties of iron-nitrogen-carbon (FeN 4 /C) catalysts via the incorporation of the boron (B) atom for achieving improved catalytic activity in oxygen electrocatalysis. Our theoretical results revealed that B modulation effectively tunes the d-band center of the iron (Fe) active site to optimize its adsorption strength with oxygenated species, greatly enhancing oxygen reduction reaction (ORR) and oxygen evolution reactions (OER) activity. Our experimental measurements then confirmed the above theoretical predictions: the as-synthesized B-doped FeN 4 /C (Fe-N 4 -B) material can perform as an eligible bifunctional catalyst for ORR and OER in alkaline media, and its catalytic activity even outperforms the commercial noble metal benchmarks. The present findings provide a promising strategy to further design the advanced catalysts for a wide range of electrochemical applications.
研究领域:
材料科学
·
电化学
·
催化
✓ 已验证
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）