INORGANIC CHEMISTRY
·
2024
·
IF 4.3
Yu Gu,Zhiqiang Tao,Shujia Zhang,Xiaohui Wang,Hao Yan,Xinmei Liu,Lei Wang,Jun Xu,Hui Shi
Methane–propane coaromatization (MPCA) upgrades two abundant and inexpensive light alkanes into value-added aromatic products. While Ga-loaded MFI zeolites represent by far the most promising catalysts for MPCA reaction, they often contain a sizable portion of Ga species at the external surface of zeolites, which are remote from the Brønsted acid sites (BAS) within MFI pores and thus inefficient for MPCA. Here, we show that Ga can be introduced into MFI pores at fairly high loadings via a simple cocrystallization approach, yielding catalysts possessing well-dispersed Ga sites predominantly residing inside the pores and framework. Adjacency between Ga and BAS within the constraints of MFI channels makes these (Ga, Al)-H-MFI catalysts more active toward methane and propane activation and more selective toward aromatics compared to the Ga/MFI counterparts prepared by impregnation that inevitably leaves a large fraction of Ga at the external surface (i.e., without confinement and few adjacent BAS). Further, the effects of the Si/Al ratio on MPCA performance have been investigated for (Ga, Al)-H-MFI catalysts. Due to the multifold roles of BAS in the overall reaction sequence, an increased BAS concentration generally results in higher propane conversion and productivity of aromatics together with lower net methane conversion and severer coking.
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2023
·
IF 7.4
Kezhen Qian,Wenmin Tian,Siwei Yan,Wentao Li,Lijie Yin,Derun Guo,Zixu Yang,Dezhen Chen,Yuheng Feng
The effects of pretreatment and structure of zeolite on aromatization of high-density polyethylene (HDPE) and polypropylene (PP) over different Ga-promoted zeolites (HZSM-5, hierarchical HZSM-5, HY, Hβ, and USY) were investigated. Hydrogen reduction of Ga-promoted HZSM-5 resulted in a higher yield of alkenes during HDPE pyrolysis but did not lead to increased production of total aromatic hydrocarbons. The reduction and subsequent oxidation of Ga/Z5 led to the formation of GaO + species with high dehydrogenation activity. This resulted in a remarkable 65% yield of aromatics, with a BTEX (benzene, toluene ethylbenzene and xylene) overall yield of 60% and a selectivity of 90% of the liquid product. Increasing the Ga loading decreased the BTEX yield due to pore blockage and a decrease in the amount of Brønsted acid sites. The BTEX yield over Ga-promoted zeolites was found to be strongly related to the pore size of the zeolite, whereas its yield over the parent zeolite was not strongly dependent on the pore size. Diffusion of the cracking intermediates was found to have a more significant impact on the aromatization of PP than HDPE. The highest BTEX yield for HDPE was achieved with Ga-promoted HZSM-5, while Ga-promoted hierarchical HZSM-5 exhibited the highest BTEX yield for PP. Furthermore, Ga(1)/Hβ-Redox demonstrated remarkable selectivity (90%) towards ethylene and propylene in the gas phase, surpassing other zeolites (37%-68%).
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
·
IF 8.758
Yanlin Zhang,Chaowei Jia,Quan Kong,Nanyu Fan,Gang Chen,Hongtao Guan,Chengjun Dong
The development of acetone gas sensors is desirable but challenging for both air quality monitoring and medical diagnosis. Herein, starting from bimetallic In/Ga metal–organic frameworks (MOFs) (MIL-68 (In/Ga)), a facile strategy is proposed to couple with zinc ions to design In/Ga oxide (IGO)@ZnO core–shell nanotubes for efficient acetone detection. In such a heterostructure, tiny ZnO nanoparticles are closely decorated on IGO nanotubes, which is beneficial to enlarge the specific surface area and create rich oxygen vacancies and heterojunction interfaces. Benefiting from the structural merits and synergetic effects, the IGO@ZnO-based gas sensor exhibits a low detection limitation (200 ppb), a high response, good linearity relationship between the sensing responses and wide testing acetone concentrations, and fast response and recovery time (6.8/6.1 s) with good selectivity and stability. These sensing performances strongly indicate the practical application to quantitatively detect acetone.
研究领域:
材料科学
·
传感器技术
·
医学诊断
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2013
·
IF 2.04
Yong Xiang,Xiaokun Zhang,Shu Zhang
Sb-doping has been demonstrated to be a new approach to promote Cu(In,Ga)Se 2 (CIGS) thin film formation . To study the mechanism of Sb-promoted CIGS formation, we investigated the influence of Sb on the evolution of the critical intermediate Cu–Se phases, and found that Cu 3 SbSe 3 species was formed. Phase change of the as-prepared Cu–Se compounds at elevated temperature was determined using the differential scanning calorimetry analysis. For samples containing Sb, the melting decomposition occurred at 507.1 °C, along with aggregation of nanocrystals into a bulk, while the morphology of the sample without Sb barely changed after heating. This result suggests that the mobile Cu 3 SbSe 3 is likely the key intermediate responsible for Sb-promoted CIGS formation. Furthermore, we extended the scope of Sb-doping approach to solvothermal synthesis and CIGS nanocrystals were synthesized with significantly promoted kinetics in the presence of Sb. Based on these results, we propose the mechanism of Sb promoted CIGS formation.
研究领域:
材料科学
·
太阳能电池
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-13
·
IF 15.7
Wang Haifeng,Lin Chao,Tan Lei,Shen Jing,Wu Xiaotong,Pan Xiangxiang,Zhao Yonghui,Zhang Haojie,Sun Yu,Mei Bingbao,Um Han-Don,Xiao Qi,Jiang Wan,Li Xiaopeng,Luo Wei
Advancements in proton-exchange membrane water electrolyzer depend on developing oxygen evolution reaction electrocatalysts that synergize high activity with stability. Here, we introduce an approach aimed at elevating oxygen evolution reaction performance by enhancing the spatiotemporal coordination of oxygen radicals to promote efficient O-O coupling. A dense, single-atom configuration of oxygen radical donors within interconnected RuO 2 nanocrystal framework is demonstrated. The stable oxygen radicals on gallium sites with adaptable Ga-O bonds are thermodynamically favorable to attract those from Ru sites, addressing dynamic adaptation challenges and boosting O-O coupling efficiency. The optimized catalyst achieves a low overpotential of 188 mV at 10 mA cm -2 , operates robustly for 800 h at 100 mA cm -2 in acidic conditions, and shows a large current density of 3 A cm -2 at 1.788 V, with stable performance at 0.5 A cm -2 for 200 h, confirming its long-term viability in proton-exchange membrane water electrolyzer applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ChemCatChem
·
2021
·Vol. 13
·期 16
·3601-3610
·
IF 5.686
Bing Xu,Minghui Tan,Xuemei Wu,Hailun Geng,Shengying Zhao,Jie Yao,Qingxiang Ma,Guohui Yang,Noritatsu Tsubaki,Yisheng Tan
Graphical Catalytic propane aromatization : Post-introducing Cr species to Ga/Z5 catalyst had the maximum dehydrogenated active Cr 3+ species. Propane was effectively converted, and more light alkenes from propane dehydrogenation were converted into BTX on 2Cr/GaZ5 catalyst. Active Cr 3+ species and strong interaction between Ga species and ZSM-5 zeolite on 2Cr/GaZ5 catalyst accelerated the dehydrogenation step in propane aromatization. Accelerating propane dehydrogenation in propane aromatization is vital because it is the first and rate control step. In this study, we introduced Cr to Ga/ZSM-5 by tuning its impregnation sequence and amount, which was expected to accelerate the dehydrogenation step and improve aromatization performance. The impregnation sequence of Cr on catalyst not only affected the interaction between Ga and ZSM-5, but also tuned the amount of dehydrogenation active species Cr 3+ . Due to the plenty of Cr 3+ species and strong interaction between Ga species and ZSM-5, 2Cr/GaZ5 catalyst accelerated the dehydrogenation step and improved the aromatization process. More light hydrocarbons were preferred to be produced and were further converted into BTX on 2Cr/GaZ5 catalyst. Excessive Cr on catalyst caused the formation of Cr 2 O 3 particles with worse dispersion. The aggregated Cr 2 O 3 decreased the strong acidity of catalyst, which could not further promote propane conversion and decreased the aromatization ability of catalyst.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
Journal of the American Chemical Society
·
2019
·
IF 14.695
Shiqun Wu,Xianjun Tan,Juying Lei,Haijun Chen,Lingzhi Wang,Jinlong Zhang
Photodriven nonoxidative coupling of CH4 (NOCM) is a potential alternative approach to clean hydrogen and hydrocarbon production. Herein, a Mott–Schottky photocatalyst for NOCM is fabricated by loading Pt nanoclusters on a Ga-doped hierarchical porous TiO2–SiO2 microarray with an anatase framework, which exhibits a CH4 conversion rate of 3.48 μmol g–1 h–1 with 90% selectivity toward C2H6. This activity is 13 times higher than those from microarrays without Pt and Ga. Moreover, a continuous H2 production (36 μmol g–1) with a high CH4 conversion rate of ∼28% can be achieved through a longtime irradiation (32 h). The influence of Ga on the chemical state of a surface oxygen vacancy (Vo) and deposited Pt is investigated through a combination of experimental analysis and first-principles density functional theory calculations. Ga substitutes for the five-coordinated Ti next to Vo, which tends to stabilize the single-electron trapped Vo and reduce the electron transfer from Vo to the adsorbed Pt, resulting in the formation of a higher amount of cationic Pt. The cationic Pt and electron-enriched metallic Pt form a cationic–anionic active pair, which is more efficient for the dissociation of C–H bonds. However, the presence of too much cationic Pt results in more C2+ product with a decrease in the CH4 conversion rate due to the reduced charge-carrier separation efficiency. This study provides deep insight into the effect of the doping/loading strategy on the photocatalytic NOCM reaction and is expected to shed substantial light on future structural design and modulation.
研究领域:
材料科学
·
催化化学
·
理论计算
✓ 已验证
产品关联
DOI
PubMed
高影响因子
MOLECULES
·
2022
·Vol. 27
·期 11
·3443
·
IF 4.927
Youjun Zhang,Licong Liu,Dixiong Yu,Jinglan Liu,Lin Zhao,Jinpeng Liu,Shuo Liu
A magnetic metal–organic framework nanocomposite (magnetic MIL-68(Ga)) was synthesized through a “one pot” reaction and used for heavy metal ion removal. The morphology and elemental properties of the nanocomposite were characterized by scanning electron microscopy (SEM), Fourier transform infrared (FT-IR), X-ray powder diffraction (XRD), as well as zeta potential. Moreover, the factors affecting the adsorption capacity of the nanocomposite, including time, pH, metal ion type and concentration, were studied. It was found that the adsorption capacity of magnetic MIL-68(Ga) for Pb2+and Cu2+was 220 and 130 mg/g, respectively. Notably, the magnetic adsorbents could be separated easily using an external magnetic field, regenerated by ethylenediaminetetraacetic acid disodium salt (EDTA-Na2) and reused three times, in favor of practical application. This study provides a reference for the rapid separation and purification of heavy metal ions from wastewater.Keywords:MOF;magnetic separation;heavy metal ions;adsorption
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
PubMed
高影响因子
MOLECULAR PHARMACEUTICS
·
2023
·
IF 4.9
Haiyan Hong,Zhihao Zha,Ruiyue Zhao,Yang Luo,Wenbin Jin,Linlin Li,Ran Wang,Li Yan,Hui Wang,Karl Ploessl,Jinping Qiao,Lin Zhu,Hank F. Kung
Fibroblast activation protein (FAP) is selectively expressed in tumors and highly important for maintaining the microenvironment in malignant tumors. Radioisotope-labeled FAP inhibitors (FAPIs) were proven to be useful for diagnosis and radionuclide therapy of cancer and are under active clinical investigations. Ga-HBED complex displays a higher in vivo stability constant (log KGaL: 38.5), compared to that of Ga-DOTA (log KGaL: 21.3). Such advantage in stability constant suggests that it may be useful for development of alternative FAPI imaging agents. In this study, previously reported [68Ga]Ga-DOTA-FAPI-02 and -04 were converted to the corresponding [68Ga]Ga-HBED-CC-FAPI-02 and -04 derivatives ([68Ga]Ga-4, [68Ga]Ga-5, [68Ga]Ga-6, and [68Ga]Ga-7). It was found that substituting the DOTA chelating group with HBED-CC led to several unique and desirable tumor-targeting properties: (1) robust, fast, and high yield labeling─readily adaptable to a kit formulation; (2) high stabilities in vitro; (3) excellent FAP binding affinities (IC50 ranging between 4 and 7 nM) and improved cell uptake and retention (in HT1080 (FAP+) cells); and (4) excellent selective in vivo tumor uptake in nude mice bearing U87MG tumor. It appeared that Ga(III) chelation with HBED-CC improved the in vivo kinetics favoring higher tumor uptake and retention compared to the corresponding Ga-DOTA complex. Out of the four tested ligands the new [68Ga]Ga-HBED-CC-FAPI dimer, [68Ga]Ga-6, displayed the best tumor localization properties, and further studies are warranted to demonstrate that it is an alternative FAP imaging agent for cancer patients.
研究领域:
医学影像学
·
肿瘤学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
PHYSICA B-CONDENSED MATTER
·
2022
·
IF 2.988
Wei Zhang,Xinhui Yang,Zhiwei Qu,Zirui Liu,Youjin Zheng,Xiangmin Zhao,Xue Wang
Ga-doped ZnO (GZO) powders were synthesized by chemical coprecipitation . GZO powders were annealed in O 2 , Ar, N 2 , and H 2 atmosphere, and the effects of annealing atmosphere on their structure, optical and electrical properties were systematically studied. The results show that the optical and electrical properties of GZO powder were highly influenced by annealing atmosphere. GZO annealed in Ar, N 2 , H 2 atmosphere have excellent electrical resistivity, while GZO annealed in O 2 atmosphere has poor electrical resistivity. According to the annealing contrasted of GZO in different atmosphere, the lower resistivity of GZO is, the lower reflectivity will be. The blue shift of ultraviolet emission (385 nm) in photoluminescence of GZO is related to oxygen vacancy (V O ) and doped Ga, the blue and green emissions (around 500 nm) are originated from V O defects. The density of V O defects and the effective doping rate of Ga will be enhanced when GZO annealed in Ar, N 2 , H 2 atmosphere.
研究领域:
材料科学
·
物理学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2021
·
IF 9.127
Suwei Mou,Kai Huang,Min Guan,Xiang Ma,Jun song Chen,Yong Xiang,Xiaokun Zhang
LiCoO 2 is the dominantly used cathode material in lithium-ion batteries. However, its high-rate capacity and cyclability are limited, especially under high charging voltages, mainly due to the high Li + diffusion barrier . To solve it, we purpose a doping scheme based on two foreign elements: one is with tremendously large ionic radius and weak electronegativity , and the other one has an ionic radius slightly larger than Co, an electronegativity a little weaker than Co, and a high binding energy with O. Ba and Ga are chosen according to this criterion, and their doping effects are compared with that of La and Al. Briefly, Ba is superior to La in weakening the attraction of O 2- to Li + because of its weaker electronegativity and larger ionic radius. Meanwhile, Ga is more capable of enhancing the structural stability at high voltages than Al mainly due to its higher binding energy with O. LiCo 0.998 Ba 0.001 Ga 0.001 O 2 increases Li + diffusivity from 0.77 × 10 -14 to 1.06 × 10 –13 cm 2 ∙s -1 , resulting in a significantly enhanced rate capacity of 114.3 mAh g -1 at 10 C, much better than pristine counterpart (1.6 mAh∙g -1 ). Additionally, it exhibits a particularly high capacity of 199.3 mAh g -1 , and 85% capacity retention over 100 cycles at 0.5 C in 3.0–4.5 V.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
LUMINESCENCE
·
2025
·Vol. 40
·期 5
·e70177
·
IF 3
Ruihao Huang,Song Ye,Meiyan Wang,Ling Pan,Tianning Zheng,Deping Wang
The manipulation of silver nanoclusters' luminescence performance in heteroatom zeolite was rarely reported. In this research, the heteroatom Ga-FAU zeolites were synthesized together with the Al FAU zeolite, based on which a series of Ag nanoclusters loaded Al FAUAg and mGa FAUAg zeolites were prepared. The spectroscopy characterization indicated that emission intensity of silver nanoclusters is greatly enhanced in Ga-containing zeolites compared to that in Al FAUAg, and meanwhile, the excitation and emission peak showed redshift and blueshift, respectively, with the introduction and increasing proportion of Ga atoms in mGa FAUAg. The TD-DFT method was carried out on the [Ag 3 Ga x D6r] + (x = 0, 1, 2, 3, 4, 5) clusters to study the effect of framework Ga on the luminescence properties of Ag 3 + in the D6r cavity of FAU zeolite, which suggested that the S 1 → S 0 transition of Ag 3 + is responsible for the radiative visible emission. Moreover, the low-energy shift for S 3 → S 0 transition and high-energy shift for S 1 → S 0 transition were observed with increasing x value in [Ag 3 Ga x D6r] + clusters, which is in accordance with the experimental observation. This research provided an alternative method for the manipulation of silver nanoclusters' luminescence performance by using heteroatom zeolite, which contributed to the design of solid phosphors with desirable emission.
研究领域:
材料科学
·
光化学
·
计算化学
✓ 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）