CRYSTENGCOMM
·
2024
·
IF 2.6
Zikun Yang,Jingxuan Zheng,shi mengge,Zhao Wang
Single-atom catalysts (SACs) have attracted significant attention due to their unique electronic structure and extraordinary catalytic reaction activity. In this work, the single-atom catalysts Au1/TiO2 were successfully prepared using cold plasma. Notably, plasma-treated TiO2 introduces a substantial number of oxygen vacancies, which played a confinement effect on gold atoms. Au1/TiO2 achieved a remarkable 67% degradation of RhB in just 120 minutes, surpassing the performance of AuNPs/TiO2 by 2.8 times. The high catalytic activity can be attributed to several factors. Firstly, plasma-treated TiO2 contained a higher density of oxygen vacancies and exhibited a narrower band gap, which improved light absorption and facilitated the anchoring of monoatomic Au on the catalyst surface. Additionally, the single-atom Au species exhibited stronger interactions with TiO2, enhancing light absorption and charge transfer capability. Simultaneously, the presence of SACs on the catalyst surface increased the number of active sites, promoting efficient separation of electron-hole pairs and consequently enhancing the photocatalytic degradation activity. Cold plasma technology offers a simple and environmentally friendly platform for the fabrication of SACs, opening up exciting possibilities for catalytic applications.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
IONICS
·
2023
·Vol. 29
·期 5
·1991-2003
·
IF 2.8
Yuhui Cui,Jinghao Lu,Lijuan Yang,Zheng Hao,Runjin Wu,Qian Li,Shijia Xu,Libin Yang
In proton exchange membrane fuel cells (PEMFCs), the most advanced catalysts are mainly carbon loaded with platinum (Pt), but the cathodic catalytic active center is too low to match the oxidation activity and rate at the anode. Co atoms doped into the lattice of Pt alloy change the electronic structure of platinum and reduce the binding energy of oxygen atoms. Au or Rh atoms embedded into the lattice of Pt 3 Co alloy compensate the defect and enhance the activity and rate of the oxygen reduction. Through base on density functional theory (DFT), the adsorption energy for oxygen on Pt 3 Co, Au-Pt 3 Co, and Rh-Pt 3 Co and the segregation energy of Co atoms were calculated. The results show that Au or Rh doped weakens the binding energy of Pt for oxygen on the Pt 3 Co alloy and improves the activity and stability of oxygen reduction. Compared with Rh, the introduction of Au element shows better effects in the electrocatalytic reaction process. Graphical Abstract
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
MICROCHEMICAL JOURNAL
·
2023
·
IF 4.8
Yanan Li,Peilin Wang,Yixin Nie,Qiang Ma
In this work, a novel sensing interface has been constructed based on the confined gold atoms-MXene nanosheet. In order to improve the sensing performance of MXene, high photoelectric active confined gold atoms-MXene nanosheet were prepared as electrochemiluminescence (ECL) emitter unit firstly. Based on the electronic metal − support interaction, gold single atoms confined on MXene can provide more active sites and efficient electron transfer to generate strong luminescence signal. Furthermore, in order to improve the biocompatibility, an ECL sensing interface with the Au atoms-MXene nanosheet and chitosan was constructed via the layer-by-layer self-assembly (LBL). Therefore, the proposed sensing interface possessed the large specific surface area, good biocompatibility, high electrocatalytic activity and strong ECL signal. As a potential biomarker, the elevated myeloperoxidase (MPO) concentration and activity were associated with many pathological factors to assess the risk of respiratory diseases. To expand the application of this ECL sensing interface in clinical diagnosis, MPO activity was detected in saliva samples. The satisfactory results indicated the confined gold atoms-MXene-based sensing interface possessed great potential in the ECL research and clinical analysis.
研究领域:
生物传感器
·
医学诊断
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Chunmei Li,Pingfan Zhang,Fang Gu,Lei Tong,Jizhou Jiang,Yan Zuo,Hongjun Dong
A new Au-θ-Al 2 O 3 /Au/PCN hybrid is fabricated by the collaborative design strategy of active site and assembled structure, which achieves highly efficient photocatalytic CO 2 reduction (CO 2 R) performance. The energy band structure of PCN is adjusted significantly owing to the strong coupling effect of Au-θ-Al 2 O 3 /Au nanosheets intercalated in PCN nanosheets. The result brings about up-shift of CB, VB and Fermi energy level overall and decrease of bandgap, which is in favor of harvesting visible light, exciting VB electrons and increasing reduction ability. In addition, the multiple built-in electric fields are induced by electron diffusion effect between structural units, due to the tight interface contact in the Au-θ-Al 2 O 3 /Au/PCN hybrid, which can effectively promote the separation of photoinduced charge carriers. Furthermore, the atomically dispersed Au atoms confined by the oxygen vacancies in Au-θ-Al 2 O 3 /Au can provide the plenty of effective active sites for CO 2 R reaction, and meanwhile, the localized surface plasmon resonance (LSPR) effect induced by Au nanoparticles on Au-θ-Al 2 O 3 /Au can improve the visible light response and produce abundant hot electrons to contribute to CO 2 R reaction. As a consequence, the average CO evolution rate of over the optimizing 10 %-Au-θ-Al 2 O 3 /Au/PCN hybrid (7.76 μmol g -1 h −1 ) reaches up to 3.53 times than that of PCN (2.20 μmol g -1 h −1 ) in the CO 2 R reaction, and maintains basically stable operation within 7 cycles of running, suggesting the superior activity and recyclability.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2025
·
IF 13.1
Xinping Duan,Yuxin Zhao,Hung-Lung Chou,Jiachang Zuo,Ruixin Wang,Weizhou Jiao,Huihuang Fang,Yanping Zheng,Haiqiang Lin,Linmin Ye,Youzhu Yuan
Metals atomically anchored on oxides have actively realized ultimate atom efficiency. However, a “molecular cork” effect causes the intrinsically reactive sites to remain dormant in various important catalytic processes. Here, we report a strategy to waken dormant atomic Au on cobalt-doped CeO2 islands (Au/CoCeO2) that are typically recognized as barely active in acetylene hydrochlorination by precisely controlling reversible C2H2 spillover facilitated by porous carbon materials, igniting its reactivity of Au-oxo sites and enhanced stability. In this vein, the C2H2 coverage on the nitrogen-doped carbon (NC) surface reversibly spills over onto HCl-corked metal sites, uncorking the strongly bound HCl. The Au/CoCeO2 + NC system displays a 2 orders of magnitude higher activity than modular Au/CoCeO2 and obtains an enhanced catalytic activity and durability than the state-of-the-art catalyst, Au/NC. This contribution unveils a distinct Eley–Rideal-like mechanism that exists on the Au/CoCeO2 + NC system, exchanging the conventional Langmuir–Hinshelwood pathway dominated over Au/NC. Collectively, our findings reinforce the importance of taming the reaction pathways for advancing catalyst design.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ChemNanoMat
·
2020
·Vol. 6
·期 8
·1191-1199
·
IF 3.384
Huixiang Li,Changhui Liang,Pan Gao,Guangjin Hou,Kairui Liu,Wei Liu,Qike Jiang,Shi Bai,Z. Conrad Zhang
Graphical In stock : Stock solutions of reduced mononuclear M 1 (0) (M=Pt, Au) atoms are prepared from their chloride salt precursors in removable solvent glycol ether/ethanol/H 2 O. Glycol ether and HCl function as strippable shields prevent M 1 (0) atoms from aggregation. The releasable M 1 (0) atoms suit as building-blocks for designable bottom-up material fabrications. Specifically, M 1 (0) atoms are readily transported onto the TiO 2 surface and remain in the reduced mononuclear state. Premade and readily transportable mononuclear zero-valent metal atoms in stock solvents offer the potential capability for bottom-up designable metallic material fabrication. This work demonstrates a potentially universal and practical strategy to prepare weakly shielded mononuclear metal atoms in a volatile solvent, which also constitutes a strippable ligand to the metal atoms. Herein, M 1 (0) (M=Pt, Au) atoms are prepared by reducing H 2 PtCl 6 and HAuCl 4 with ethanol in ethylene glycol diethyl ether (EGDE) under mild temperatures. The diether oxygens of EGDE, H + , and Cl − coordinating to the M 1 (0) atoms, make the M 1 (0) atoms stable in the solvent under low pH. However, the M 1 (0) atoms can be released either by evaporation of HCl and EGDE or through neutralization of the HCl with a base. The premade M 1 (0) atoms can be used as primary building blocks to construct designable materials. To demonstrate a potential application, the M 1 (0) atoms are conveniently transported onto the surface of TiO 2 through impregnation followed by mild heating. The atomic dispersion and reduced state of the metal atoms are well preserved, as verified by HAADF-STEM images, XPS, and DRIFT spectroscopy.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2021
·
IF 6.986
Jinna Guo,Mingsen Xie,Peiyao Du,Yu Liu,Xiaoquan Lu
Luminol, as a classical luminophore, plays a crucial role in electrochemiluminescence (ECL). However, the traditional luminol–H2O2 ECL system suffers from the self-decomposition of H2O2 at ambient temperature, which hinders its further application in quantitative analysis. In this work, for the first time, we developed atomically gold-supported two-dimensional VO2 nanobelts (Au/VO2) as an advanced co-reaction promoter to speed up the reduction of dissolved oxygen to superoxide radicals (O2•–), which react with the luminol anion radical and greatly promote the ECL emission. The ECL resonance energy transfer (ECL-RET) between the hollow manganese dioxide nanospheres and luminol results in a conspicuously decreased ECL signal response, and in the presence of glutathione (GSH), effective redox reaction between manganese dioxide and GSH restores the ECL signal. As a consequence, the designed sensor based on ECL-RET-assisted Au/VO2 signal amplification showed outstanding performance for “signal-on” detection of GSH in the concentration range of 10–3 to 10–10 M, and the detection limit was as low as 0.03 nM. The ECL sensor displayed excellent specificity and was successfully utilized to target GSH in real human serum samples. Importantly, this work not only highlights a powerful avenue for constructing an ultrasensitive ECL sensor for GSH but also provides some inspiration for the further design of high-performance co-reaction accelerators using the ECL technique.
研究领域:
分析化学
·
生物传感
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2022
·
IF 9.965
Yongbin Wu,Shaobo Han,Yong Li,Wenjie Shen
Monodisperse gold-copper nanocubes and AuCu-cuprous sulfide (Cu 1.96 S) heterodimers were fabricated by a step-wise polyol reduction with the aid of oleylamine and 1-dodecanethiol. The geometric configuration was mediated by simply varying the Cu/Au atomic ratio: Au-Cu cubes with sizes of 6.4 and 4.3 nm were yielded at Cu/Au atomic ratios of 1/3 and 1/1, respectively; while AuCu-Cu 1.96 S heterodimer, consisting of a AuCu cube of 4.6 nm and a Cu 1.96 S sphere of 6.3 nm was obtained at Cu/Au atomic ratio of 3/1. Detailed structural analysis on the intermediate products, collected at different intervals during the synthesis, revealed that small-sized Au seeds formed at 423 K, followed by the growth of Cu and Cu 1.96 S crystals at 473 K. Oleylamine coordinated to Au 3+ and Cu 2+ and thus mediated the particle size; while 1-dodecanethiol bonded to Au 3+ and directed the cubic morphology. Excessive Cu 2+ , at the Cu/Au atomic ratio of 3/1, interacted with 1-dodecanethiol and formed Cu 1.96 S spherical particle that epitaxially grew over the AuCu cube, resulting in a heterodimer structure. Due to the enriched surficial Cu atoms and their electronic interactions with Au atoms, Au-Cu nanocubes and AuCu-Cu 1.96 S heterodimers showed pronounced activities for the catalytic reduction of 4-nitrophenol to 4-aminophenol with NaBH 4 at 298 K.
研究领域:
材料科学
·
纳米技术
·
化学工程
·
催化
✓ 已验证
DOI
PubMed
高影响因子
Materials Today Nano
·
2024
·
IF 8.2
Jiangyong Li,Qin Li,Qian Yang,Qi Tang,Xiaoyi Hu,Qing Liu,Liangke Zhang
Reactive oxygen species (ROS)-based antitumor strategies, particularly chemodynamic therapy, have garnered considerable attention. However, challenges such as difficulties in achieving deep penetration, relatively low H 2 O 2 levels in the tumor microenvironment, the requirement for low pH by the Fenton reaction, and their short lifespan have impeded satisfactory therapeutic outcomes. Hence, we have developed a nanoplatform with enhanced permeability that not only generates significant amounts of ROS but also converts them into longer-lasting reactive nitrogen species (RNS), thereby improving tumor therapy efficacy. In our study, carbon dots were functionalized by doping with gold atoms and grafting nitrosoglutathione (GSNO) to form ACN, which exhibits glucose oxidase-like properties and enables laser-responsive NO release. ACN and indocyanine green (ICG) were then loaded onto MnO 2 nanoflowers to form MnO 2 @AI. Upon arrival at the tumor site, MnO 2 reacts with H 2 O 2 and GSH, leading to its degradation and the subsequent release of ACN, which is characterized by three permeation-promoting properties: ultra-small size, positive charge, and NO content. In addition, ACN promotes H 2 O 2 production through glucose metabolism and reduces pH, both of which enhance the Fenton-like reaction of MnO 2 , thereby amplifying ROS generation. The ICG in MnO 2 @AI enhances its photothermal properties, leading to the responsive release of NO from GSNO grafted onto ACN, which then reacts with the increased ROS to generate more toxic RNS. Collectively, the approach described herein offers substantial potential for advancing the treatment of malignant tumors.
研究领域:
纳米技术
·
癌症治疗
·
材料科学
·
生物医学工程
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Xiangzhan Meng,Yongqiang Zhang,Zengxi Li,Hui Wang,Suojiang Zhang
Au supported on monoclinic ZrO2 (Au/m-ZrO2) prepared by deposition–precipitation method showed excellent catalytic performance in the aerobic oxidation of amino alcohols to amino acids, i.e., glycine, alanine, serine, β-alanine, and 2-aminobutyric acid. The Au particle size and valence distribution of the gold species were adjusted by calcination temperature, as demonstrated by XRD, TEM, UV–vis DRS, XPS, and H2-TPR, which significantly influenced the catalytic activity but not the selectivity of amino acids. Metallic gold atoms on the surface were shown to be the active sites by the correlation between reaction rate per mole of metallic Au and Au particle size. The kinetics of oxidation of monoethanolamine (MEA) was studied in detail, and the results indicated that MEA oxidation is a first-order reaction with an activation energy of 52.8 kJ·mol–1.
研究领域:
催化
·
化学工程
·
材料科学
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）