FUEL
·
2023
·
IF 7.4
Siqi Wu,Rong Guo,Jianshan Chen,Runping Ye,Yeyan Qin,Hanying Wu,Shanshan Zong,Yang Liu,Yuangen Yao
Lack of high performance and stability catalysts remains a technical bottleneck for the industrialization of methyl nitrite (MN) carbonylation to dimethyl carbonate (DMC). Lewis acidity is crucial for catalytic performance in MN carbonylation reaction, but the regulation of Lewis acid sites and the effects of Lewis acid strength on catalytic performance have not been clarified. Thus, rational design of NaY zeolites with controllable acidity is an effective strategy to promote their catalytic performance. Herein, we substituted Ga for partial framework Al to produce a series of NaGaY-x (x = 0 ∼ 2) zeolites with different Ga content via direct hydrothermal method and applied in this reaction. The results showed that the Lewis acid strength increased upon an appropriate amount of Ga incorporation, thereby the electron density of Pd 2+ could be regulated. The optimal electron density of Pd 2+ promotes the carbon monoxide (CO) adsorption and activation, which contribute to the formation of the critical intermediate species *COOCH 3 . Eventually, the Ga-modified PdCu/NaY catalyst exhibited remarkable catalytic activity for MN carbonylation to DMC with the weight-time yields (WTY DMC ) of 1251 g·kg cat −1 ·h −1 , and the CO conversion to DMC (C CO ) of 69.2 % as well as the DMC selectivity based on CO (S DMC/CO ) up to 100 %. Our work paves the way to further understand the synergistic effect between Pd 2+ and Lewis acid, assists in the development of high-performance MN carbonylation catalysts.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Cheng Huang,Kun Li,Hong Zhang,Wenwen Zhang,Yanlin Sun,Shujie Xing,Ying Shao,Jing Zhu,Yalan Chen,Long Chen
In this study, a solid adsorbent based on Chinese gallotannin and chitosan was generated and applied to adsorb rare and scattered metals, including Ge (Ⅳ), Ga (Ⅲ), and In (Ⅲ), from simulated zinc plant leachates. Fourier-transform infrared spectroscopy (FTIR) and solid state nuclear magnetic resonance (SSNMR) were performed to characterize the grafting way of Chinese gallotannin on the chitosan matrix. It was clearly showed that Chinese gallotannin was immobilized on the chitosan by Schiff-base condensation and phenol-formaldehyde reaction at the molar ratio of glutaraldehyde to tannin of 2:1. And the amount of chitosan amino groups was ten times that of tannin, with an initial pH of 4. The adsorption experiments showed that an appropriate increase in pH was more beneficial to enhance the adsorption capacity of immobilized Chinese gallotannin (ICGT). At a temperature exceeding 30 °C, the immobilized tannin became less sensitive to temperature. Adsorption kinetics studies showed that the adsorption of the three scattered metals by ICGT followed a quasi-second-order kinetic equation , with chemisorption as the mechanism. The adsorption isotherm was well fitted by the Langmuir model, indicating uniform adsorption sites on the surface of ICGT. The adsorption capacities of Ge (Ⅳ), Ga (Ⅲ), and In (Ⅲ) in solution by the adsorption model of monolayer were 61.39 mg/g, 63.82 mg/g, and 59.92 mg/g, respectively. Mechanical property and stability tests showed that ICGT had good resistance to harsh adsorption conditions of scattered metal ions .
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Manman Zhang,Xiaopei Zhang,Chang Liang,Lei Qin,Dongju Fu,Meiling Wang,Yonghui Bai,Weifeng Liu,Xuguang Liu
To meet the requirements of Ga(Ⅲ) selective adsorption from acid leaching of fly ash, a grapheme-based Ga(Ⅲ) imprinted polymer is developed by combining adsorption method with surface ion imprinting technology. The obtained Ga(Ⅲ) imprinted polymer can effectively adsorb Ga(Ⅲ) with a maximum adsorption capacity of 221.56 mg g −1 at an initial concentration of 200 mg/L within 240 min. The pseudo-second order model (R 2 = 0.9882) and Langmuir isotherm (R 2 = 0.9628) fitted the Ga(Ⅲ) adsorption data well. In addition, the imprinted adsorbent exhibits significant selectivity towards Ga(Ⅲ) in a simulated acid leaching of fly ash. The selectivity coefficients of Ga(Ⅲ) with respect to Al(Ⅲ), Fe(Ⅲ), Mg(Ⅱ), and Ca(Ⅱ) are 10.09, 3.36, 18.50, and 55.50, respectively. The synthesized imprinted adsorbent exhibits excellent regeneration ability, maintaining 85.71% of its initial adsorption capacity after 5 adsorption-regeneration cycles. The binding energy of Ga(Ⅲ) to functional monomers is calculated as −16.79 kJ mol −1 , which confirms that Ga(Ⅲ) can be effectively adsorbed. The theoretical simulated calculation results are basically in consistence with the experimental results, which confirms the selective adsorption mechanism of Ga(Ⅲ). Therefore, it provides a new idea for the extraction of Ga(Ⅲ) from acidic environments.
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ACS Applied Materials & Interfaces
·
2023
·
IF 9.5
Peng Wang,Baoluo He,Xiaozhi Zhang,Shujuan Liu,Qian Ye,Feng Zhou,Weimin Liu
In this study, size-regulated MOFs (MZ) with high MBT loading were successfully synthesized by combining mercaptobenzothiazole (MBT), zinc salt, and 2-methylimidazole (2-MI). Subsequently, the MZ structure was utilized to encapsulate tannic acid-modified gallium-based liquid metal (GLM-TA), thereby acquiring a novel heterogeneous nanocomposite (GLM-TA@MZ). The results revealed that the as-prepared GLM-TA@MZ shows good antiwear and friction-reducing performance as an oil-based lubricant additive, the average friction coefficient was decreased to 0.091, and a wear volume was reduced to 0.95 × 104 μm3, which corresponds to a decrease of 52.3 and 97.2% as compared to base oil PAO. The excellent tribological properties of GLM-TA@MZ can be attributed to physical adsorption on the friction pair, followed by tribochemical reactions. As a result, a thick friction protection film (thickness of about 100 nm) containing Ga, Zn, and S elements was formed, which effectively reduced the contact area between the friction pairs, resulting in improved tribological performance. This study provides insights into the design of MOF-based nanocomposites for lubricating applications.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Tingzhan Wang,Jingkun Chen,Jiaxuan Chen,Xuan Yao,Gang Chen,Zheng Jiao,Jing-Tai Zhao,Shuai Cheng,Xue-Chun Yang,Qianli Li
N-butanol gas is a common volatile organic compound (VOC) that can pose a threat to human health and pollute the atmospheric environment. However, the n-butanol gas sensors suffer from low response and selectivity. Herein, we synthesized the Ga-doped ZnO (ZOG) sensors by one-step hydrothermal treatment and subsequent calcination. The oxygen vacancies content of 1-ZOG has increased by 46 % compared to pure ZnO. Rich oxygen vacancies can increase the response signal of 1-ZOG to 174.78 in darkness for 100 ppm n-butanol, which is 2.4 times that of ZnO. Furthermore, the gas sensing performance of 1-ZOG is improved by light excitation. Under UV irradiation, the response of 1-ZOG sensor to 100 ppm n-butanol is 3.6 times that of pure ZnO, up to 636.81. Meanwhile, the response signal of 1-ZOG to n-butanol is at least 6.32 times that of other gases under UV light, showing ultra-high selectivity. This study proved that both Ga doped and photo-excited are effective strategies for improving the sensitivity and selectivity of ZnO based gas sensors.
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APPLIED SURFACE SCIENCE
·
2021
·
IF 6.707
Girma Sisay,Hairus Abdullah,Dong-Hau Kuo,Worku Lakew,Hardy Shuwanto,Sleshi Fentie
The works on photocatalytic hydrogen production and green chemical conversion have received significant attention due to the current need for clean energy and a secure environment. Herein, Ce and Ga codoped Zn(O,S) has been synthesized with different amounts of Ce using facile precipitation method at a low temperature of 95 °C and characterized by XRD, SEM, HRTEM, XPS, EPR, Raman, DRS, PL, EIS, UV–vis, GC–MS, and photocurrent response measurements. The as-prepared photocatalysts were utilized for hydrogen production and hydrogenation of toxic organic compounds, viz. nitrobenzene (NB) and azobenzene (AB) into a valuable product of aniline. The incorporation of Ce and Ga into Zn(O,S) enhanced the hydrogen evolution and hydrogenation reactions of NB and AB. This notable enhancement was ascribed to the synergistic effects of Ce and Ga dopants to form positively charged defects that trap the photogenerated electron. The trapping mechanism improves the photogenerated charge separation and transfer as confirmed with impedance spectroscopy (EIS), transient photocurrent response, and PL measurements. The highest hydrogen production was attained by 15Ce-5Ga-Zn(O,S) with a rate of 7130 μmol∙g − 1 ∙h − 1 in 10% ethanol solution. In addition, NB and AB were effectively converted to aniline in 15 min and 30 min, respectively. A plausible photocatalytic hydrogenation mechanism for both hydrogenation of NB and AB is proposed with the steps of surface adsorption, molecular diffusion, pinning at oxygen vacancy sites, and hydrogenation reaction with the help of in situ generated H + coupled with electrons.
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DALTON TRANSACTIONS
·
2021
·Vol. 50
·期 42
·15057-15061
·
IF 4.39
Ming-Yang Cao,Chun-Li Hu,Fang Kong,Zhe-Yao Xiong,Jiang-Gao Mao
Exploration of new types of borates is important because of their promising applications in diverse fields. Two new boroselenites, namely, M(B(SeO3)3)H2O (M = Al, Ga), which represent the first IIIA metal boroselenite, were synthesized by hydrothermal reactions. M(B(SeO3)3)H2O (M = Al, Ga) possesses a unique sandwich like double-layer structure formed by two 2D [MSe2O8]5− layers interconnected by 1D [BSeO5]3− chains. More interestingly, both compounds display large band gaps (4.86/4.79 eV) and moderate birefringences (Δn = 0.063/0.064 at 1064 nm) based on density functional theory (DFT) calculations.
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Catalysis Science & Technology
·
2019
·Vol. 9
·期 11
·2812-2827
·
IF 5.726
Suyao Liu,Yurong He,Huaike Zhang,Zhiqiang Chen,Enjing Lv,Jie Ren,Yifeng Yun,Xiaodong Wen,Yong-Wang Li
Ga-Doped ZSM-22 zeolites were synthesized successfully via a hydrothermal method by directly incorporating Ga species into the zeolite framework. It appeared that the as-prepared Ga-substituted zeolites possessed high crystallinity, uniform morphology and open pore structure. The XRD, FTIR, XPS as well as 71Ga and 29Si MAS NMR results confirmed the presence of Ga species in the framework of zeolites and the formation of the Ga–OH–Si group, thus leading to a significant decrease of Brønsted acidity because of the lower acidity of the Ga–OH–Si bridge hydroxyl compared to that of the Si–OH–Al group. These characteristics ensured that the Pt-loading [Al, Ga]-ZSM-22 catalyst exhibited lower cracking activity and higher selectivity (about 78.2% at 90.5% of conversion) in the n-dodecane isomerization than the parent Pt/ZSM-22 catalyst, due to the more balanced bifunctionality between acid sites and metal sites. DFT calculations revealed that Al and Ga incorporation was mostly prevalent at the T2, T3 and T4 sites, while Fe heteroatom substitution occurred equivalently in four sites. Bader charge analysis suggested that the acidity decreased in the order of Al-ZSM-22 > Ga-ZSM-22 > Fe-ZSM-22, and the cracking activity exhibited the order of Al-ZSM-22 ≫ Ga-ZSM-22 > Fe-ZSM-22. Therefore, it could be concluded that the isomerization was facilitated by the combination of the heteroatom location and the acidity strength. Remarkably, no significant decline of crystallinity and special surface area of Ga-doped zeolites was observed after the high temperature calcination, revealing higher stability of Ga than Fe in the zeolite framework.
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JOURNAL OF SOL-GEL SCIENCE AND TECHNOLOGY
·
2018
·Vol. 86
·期 3
·699-710
·
IF 1.745
Guo Jiuli,Han Qiuwan,Zhong Siyuan,Zhu Baolin,Huang Weiping,Zhang Shoumin
The M-modified TiO 2 nanotubes (NTs) (M = Ce, Ga, Co, Y, 2.0 wt%) were synthesized by combining sol-gel method with hydrothermal treatment, based on which gold was loaded by the deposition–precipitation approach. These catalysts were loaded with 1.5 wt% gold and calcined at 300 °C, and their catalytic performance was compared with Au/TiO 2 NTs in CO oxidation. TEM results manifested Au/M-TiO 2 NTs (M = Ce, Ga, Co, Y) had smaller gold nanoparticles than Au/TiO 2 NTs. Patterns of XPS revealed the presence of the strong interaction between gold and support in Au/M-TiO 2 NTs (M = Ce, Ga, Co, Y). Ce 4+ , Ga 3+ , Co 2+ , and Y 3+ ions were present as CeO 2 , Ga 2 O 3 , CoO, and Y 2 O 3 in Au/M-TiO 2 NTs (M = Ce, Ga, Co, Y), respectively. Based on O 2 -TPD studies, Au/M-TiO 2 NTs (M = Ce, Ga, Co, Y) provided new O 2 adsorption sites for the adsorption and activation of oxygen in CO oxidation. M (M = Ce, Ga, Co, Y) modifying performed the positive effect on CO oxidation activity and Au/Y-TiO 2 NTs showed the highest activity among these catalysts. Additionally, Au/Y-TiO 2 NTs also performed excellent high-temperature stability. It was likely that the strong interaction between gold and support created the small size of gold nanoparticles, large O 2 adsorption and plenty of defects, thereby enhancing the catalytic activity of Au/M-TiO 2 NTs (M = Ce, Ga, Co, Y).
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Qihua Liang,Guotao Lin,Junting Gao,Zequan Li,Qingge Feng
Formaldehyde is a ubiquitous indoor pollutant. Developing metal oxide semiconductors gas sensors for selective ppb-level formaldehyde detection is challenging. Therefore, developing gas sensors that can selectively detect indoor formaldehyde at ppb levels is important. In this study, outer-walled thin sheet-like microspheres of Ga-doped In 2 O 3 (Ga x In 2-x O 3 , x = 0, 0.1, 0.2, 0.3, and 0.4) were fabricated using a facile two-step synthetic method. The Ga 0.3 In 1.7 O 3 based sensor shows the response (556 ± 25) to 100 ppm formaldehyde at 80 °C, which is around 6.5 times that of the pure In 2 O 3 based sensor at 90 °C. Furthermore, it has fast response time (< 3 s), excellent selectivity (S Formaldehyde /S Ethanol = 160, S Formaldehyde /S Acetone = 267), good stability (at least 60 days), and ultra-low limit of detection (10 ppb) for formaldehyde at 80 °C. The improved formaldehyde sensing performance of Ga 0.3 In 1.7 O 3 microspheres is attributed to the optimization of surface chemisorbed oxygen, which is caused by Ga doping regulating the Fermi level of In 2 O 3 as well as an increase in the specific surface area.
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EUROPEAN JOURNAL OF NUCLEAR MEDICINE AND MOLECULAR IMAGING
·
2024
·
IF 8.6
Song Yangmeihui,Qin Chunxia,Chen Yixiong,Ruan Weiwei,Gai Yongkang,Song Wenyu,Gao Yu,Hu Wenzhu,Qiao Pengxin,Song Xiangming,Lv Xiaoying,Zheng Danzha,Chu Huikuan,Jiang Dawei,Yang Ling,Lan Xiaoli
Purpose The reversibility of early liver fibrosis highlights the need for improved early detection and monitoring techniques. Fibroblast activation protein (FAP) is a promising theranostics target significantly upregulated during fibrosis. This preclinical and preliminary clinical study investigated a FAP-targeted probe, gallium-68-labeled FAP inhibitor 04 ([ 68 Ga]Ga-DOTA-FAPI-04), for its capability to visualize liver fibrosis. Methods The preclinical study employed [ 68 Ga]Ga-DOTA-FAPI-04 micro-positron emission tomography (PET)/computed tomography (CT) on carbon tetrachloride-induced mice model (n = 34) and olive oil-treated control group (n = 26), followed by validation of the probe's biodistribution. Hepatic uptake was correlated with fibrosis and inflammation levels, quantified through histology and serum assays. FAP and α-smooth muscle actin expression were determined by immunohistochemistry, as well as immunofluorescence. The subsequent clinical trial enrolled 26 patients with suspected or confirmed liver fibrosis to undergo [ 68 Ga]Ga-DOTA-FAPI-04 PET/magnetic resonance imaging or PET/CT. Key endpoints included correlating [ 68 Ga]Ga-DOTA-FAPI-04 uptake with histological inflammation grades and fibrosis stages, and evaluating its diagnostic and differential efficacy compared to established serum markers and liver stiffness measurement (LSM). Results [ 68 Ga]Ga-DOTA-FAPI-04 mean uptake in mice livers was notably higher than in control mice, increasing from week 6 [0.70 ± 0.11 percentage injected dose per cubic centimeter (%ID/cc)], peaking at week 10 (0.97 ± 0.15%ID/cc) and slightly reducing at week 12 (0.89 ± 0.28%ID/cc). The hepatic biodistribution and FAP expression showed a consistent trend. In the patient cohort, hepatic [ 68 Ga]Ga-DOTA-FAPI-04 uptake presented moderate correlations with inflammation grades (r = 0.517 to 0.584, all P < 0.05) and fibrosis stages (r = 0.653 to 0.698, all P < 0.01). The average SUVmax to background ratio in the liver showed superior discriminative ability, especially between stage 0 and stage 1, outperforming LSM (area under curve 0.984 vs. 0.865). Conclusion [ 68 Ga]Ga-DOTA-FAPI-04 PET shows significant potential for non-invasive visualization and dynamic monitoring of liver fibrosis in both preclinical experiment and preliminary clinical trial, especially outperforming other common clinical indicators in the early stage. Trial registration NCT04605939. Registered October 25, 2020, https://clinicaltrials.gov/study/NCT04605939
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Journal of Materials Chemistry C
·
2024
·
IF 5.7
Ruixin Sun,Jinxing Zhao,Ouyang Lin,Yu Li,Xiulin Xie,Wentao Niu,Zhe Yin,Aiwei Tang
I–III–VI-group semiconductor nanocrystals (NCs) have received extensive attention for use in quantum-dot light-emitting diodes (QLEDs) due to their nontoxic nature, large-scale tunable emission wavelength and straightforward synthesis. At present, research on ternary CuGaSe2 (CGSe) NCs is gradually being carried out. CGSe-based semiconductor NCs with a wide and tunable bandgap exhibit significant promise for efficient QLEDs preparation. In order to improve their functionality, stability and dispersion, Zn2+ was introduced into CGSe cores, which were coated with wide-band-gap ZnS to form Cu–Ga–Zn–Se/ZnS NCs to improve their luminescence performance. In this work, a series of Cu–Ga–Zn–Se/ZnS NCs with tunable emission from 603 to 524 nm and a photoluminescence quantum yield (PLQY) of 96% could be acquired by precisely controlling the non-stoichiometric Cu : Ga molar ratios in the synthesis of the CGZSe cores. Furthermore, green luminescent CGZSe/ZnS NCs were obtained by adjusting the amount of crucial Zn precursors during nucleation and shell formation. The green QLEDs based on these NCs show a high external quantum efficiency of 5.8% and a high brightness of 7016 cd m−2. This work reveals new possibilities for the design of novel and efficient Cd-free green QLEDs.
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