JOURNAL OF CATALYSIS
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2024
·
IF 6.5
Jianxian Li,Wenting Lin,Minglei Lu,Junwei Liao,Changsong Hu,Tiejun Wang
Efficient release of H 2 with negligible CO impurities from sustainable MeOH/H 2 O has become a promising goal for on-board hydrogen generator. However, hydrogen release kinetics still face challenges. In this work, the Cu/ZnO/CeO 2 catalyst with high density ultra-small Cu nanoparticles and abundant oxygen vacancies were prepared for intensifying hydrogen evolution in aqueous phase reforming of methanol (APRM). The optimized 55% Cu/ZnO/CeO 2 catalyst (Cu NPs of 3.8 nm, Cu loading of 55.89 wt%, oxygen vacancies of 2.316 × 10 15 spins g −1 ) exhibited an excellent H 2 evolution rate of 58.39 μmolg cat −1 s −1 even at low temperature of 210 °C, which was 2.1-fold enhancement than that of commercial Cu/ZnO/Al 2 O 3 catalyst. Characterizations and experiments revealed that ZnO/CeO 2 intensified the strong metal-support interaction (SMSI), which anchored the Cu NPs, generated abundant oxygen vacancies and adjusted electronic structure to form Cu 0 -Cu + -O v active sites for facilitating the kinetics of APRM.
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Journal of Energy Chemistry
·
2017
·
IF 2.594
Ya'nan Yao,Yan Gao,Lu Ye,Hu Chen,Licheng Sun
The development of efficient molecular catalysts for visible-light driven CO 2 reduction, based on abundant materials, is necessary to meet energy demands and address environment problems. In this work, a Co(bpy) 2 Cl 2 catalyst was developed and showed high efficiency and durability for the photocatalytic reduction of CO 2 and protons. Yields of CO and H 2 as high as 62.3 and 69.9 µmol were achieved and the turnover numbers (TONs) reached 6230 and 6990, respectively, under light irradiation ( λ > 420 nm) for 4 h, indicating that the mixture gases could be a candidate as syngas . The apparent quantum yield was determined to be 2.1% for CO. Mechanistic studies revealed oxidative quenching of the photosensitizer Ru(bpy) 3 Cl 2 by the catalyst. The photocatalytic performance, flexible synthesis and non-noble metal catalyst in our system show great promise for the practical application of Co(bpy) 2 Cl 2 to photocatalytic reduction of CO 2 .
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高影响因子
IONICS
·
2025
·
IF 2.6
Lu Lianwu,Guo Shenghui,Hua Yixin,Cheng Mingqiang,Zhang Yinghua,Gao Lei,Ru Juanjian
Brightly saturated oxide films are successfully prepared on Ti sheets surface by anodic oxidation in ethaline deep eutectic solvent (DES) with the regulation of H 2 O content, to enhance the decorative and corrosion resistance. As H 2 O content increases from 0 wt .% to 100 wt .% in the DES, the colored surface of Ti sheets exhibits a highly reproducible and a variety of colors including yellow, brown, red, purple, and blue. The role of H 2 O during the coloring process is discussed to shed light on the deeper causes of the color changes of Ti sheets. There exists a critical H 2 O content, i.e. 20 wt. %, and below this value, it benefits to the increase of bath voltage and the formation of oxide films, reflecting in a regular change in the color of Ti sheets. Above 20 wt. %, some characteristics conferred by ethaline DES may be weakened, so that the color of Ti sheets basically remains unchanged in blue tone. Besides, systematically characterizations of colored Ti sheets demonstrate that non-stoichiometric titanium oxides are formed as a mixture of TiO 2 , Ti 2 O 3 and TiO. The variations in H 2 O content have significant impacts on the surface composition of colored Ti sheets, resulting in an increased O/Ti ratio of the surface oxides and altering the optical properties of the colored films. Furthermore, the EIS and dynamic potential polarization tests show a significant increase in impedance and a decrease in corrosion current density for the colored Ti sheets compared to the untreated, implying an enhancement in corrosion resistance.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3846
·
IF 4.2
Lei Huang,Jian Qian,Shijian Sun,Zheng Li,Dechuan Li
A novel method for synthesizing dumbbell-shaped (Gd1−xTbx)2O(CO3)2·H2O (GOC:xTb3+) phosphors using sodium carbonate was investigated. An amount of 1 mmol of stable fluorescent powder can be widely prepared using 3–11 mmol of Na2CO3at a pH value of 8.5–10.5 in the reaction solution. The optimal reaction conditions for the phosphors were determined to be 7 mmol for the amount of sodium carbonate and a pH of 9.5 in the solution. Mapping analysis of the elements confirmed uniform distribution of Gd3+and Tb3+elements in GOC:xTb3+. The analysis of fluorescence intensity shows that an optimal excitation wavelength of 273 nm is observed when the concentration of Tb3+is between 0.005 and 0.3. The highest emission intensity was observed for GOC:0.05Tb3+with a 57.5% maximum quantum efficiency. The chromaticity coordinates show that the color of GOC:Tb3+is stable and suitable for fluorescence recognition. Latent fingerprint visualization reveals distinctive features like whorls, hooks, and bifurcations. Therefore, the sodium carbonate method offers an effective alternative to traditional urea chemical reaction conditions for preparing GOC:Tb3+.
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PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
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2025
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IF 19
Wenchao Shangguan,Guoqiang Li,Shidi Gui,Xiaodong Zhang,Sugang Meng,Shifu Chen,Yingxuan Li
Separating photoexcited holes in metallic nanostructure to drive H 2 O oxidation reaction to balance the CO 2 photoreduction reaction is highly desirable, but challenging. The bottleneck lies in the sluggish kinetics of both photoexcited hole transfer and H 2 O oxidation. Herein, this work demonstrates that the in situ reconstruction of n -type wide-bandgap AlOOH-supported Au nanoparticle heterogeneous photocatalyst, triggered by thermal and photothermal cooperative effect during photocatalytic reactions, facilitates the efficient CO 2 photoreduction through optimizing the Au 5 d -band holes separation and H 2 O activation. In situ and ex situ characterizations evidence restructuring at interfaces to form an ultrathin γ-Al 2 O 3 nanolayer (≈2 nm thickness), which optimizes the energy band structure and promotes spontaneous transfer of photoexcited Au 5 d -band holes to the valence band of AlOOH, and prolongs the lifetime of electrons available for CO 2 reduction on Au. Furthermore, hydroxyl vacancies generated during restructuring process are demonstrated to promote H 2 O adsorption and lower the energy barrier for O 2 formation, supplying adequate protons for CO 2 protonation reduction and thereby boosting CO 2 photoreduction efficiency. This study offers valuable insights into the underlying mechanisms of utilizing n -type semiconductors to separate photoexcited d -band holes in metal nanoparticles.
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CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenhao Ding,Guolang Zhou,Xiangjie Guo,Cheng Liu,Tianshi Wang,Yongsheng Fu,Jingzhou Yin,Lili Zhang,Edison Huixiang Ang
The natural reactivity of Zn metal in aqueous environments leads to surface deterioration and uncontrolled dendrite growth, posing challenges in the advancement of Zn-ion batteries. In this research, we introduce an environmentally friendly and cost-effective electrolyte additive, ammonium oxalate (AO), to significantly extend the cycle life of Zn-ion batteries with minimal usage. Oxalate ions within AO actively participate in the solvation of hydrated Zn ions and attach to the Zn anode surface prior to H 2 O molecules, creating a robust solid-electrolyte interface (SEI) layer. This SEI layer serves a dual purpose: it inhibits further reactions with H 2 O and restricts the two-dimensional movement of Zn ions, promoting the preferential growth of the (0 0 2) crystal plane. Consequently, Zn||Zn cells exhibit an impressive lifespan surpassing 1800 h (at 1 mA cm −2 , 1 mAh cm −2 ), and Zn||Cu cells experience a tenfold increase in cycling life. Moreover, Zn||MnO 2 full cells, incorporating this low-cost and highly efficient inorganic additive, maintain an outstanding 80.84 % capacity retention after 1200 cycles at 1 A g −1 . This breakthrough with AO offers a promising avenue for the practical implementation of Zn-ion batteries, emphasizing their cost-effectiveness and environmental sustainability.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2025
·
IF 2.1
Hongyu Qi,Jiaxin Han,Lin Xing,Jia Xu,Yushan Liu,Xun Wang,Tao Zhang,Yong Ma,Lingzong Meng
The phase equilibrium of the quinary system LiCl–Li2SO4–LiBO2–Li2B4O7–H2O at 323.15 K was studied with an isothermal dissolution method. The dry-salt phase diagram of the quinary system consists of one invariant point saturated with LiCl·H2O, Li2B4O7·3H2O, and LiBO2·2H2O, three univariant curves, and three crystallization regions saturated with Li2SO4·H2O corresponding to LiCl·H2O, Li2B4O7·3H2O, and LiBO2·2H2O. The J(H2O), J(Li2SO4), refractive index, and pH value change gradually with the changing concentration. Combining the equilibrium constants for boron-containing species, the pH values, and concentration of total boron, the boron-containing species distributions in the mixed solution in the system were calculated. The concentrations of B3O3(OH)52– and B5O6(OH)4– are very low and can be neglected. The boron-containing species distributions are mainly affected by m(LiCl) in the solution but less by m(Li2SO4). The results of the phase diagram and boron-containing species distribution in the quinary system can provide fundamental thermodynamic data for the extraction of lithium borate from brines.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Shuyi He,Zheguan Lin,Jie Shi,Linyu Zhou,Qingyan Cui,Tiesen Li,Jiangyong Liu,Yuanyuan Yue
For traditional strategies to construct SO 2 and H 2 O co-resistant systems in low-temperature NH 3 selective catalytic reduction (NH 3 -SCR) catalysts, the primary challenge lies in mitigating the partial loss of redox activity at active sites. Herein, we present an approach to construct a protective system based on interface engineering principles, effectively safeguarding Cu active sites in ZnO/FeCu-SSZ-13 under SO 2 and H 2 O exposure. The core innovation stems from the creation of a strong interface effect originated from Zn-O-Al bonds formed between ZnO and the framework Al on the FeCu-SSZ-13 surface. This interface effect can regulate the electronic structure of Zn O bonds on ZnO component, producing abundant basic sites around the Cu active sites, enabling the preferential adsorption of SO 2 and its oxidation into ZnSO 4 , thereby virtually eliminating the redox ability loss of Cu active sites. As a result, ZnO/FeCu-SSZ-13 achieves exceptional low-temperature NH 3 -SCR performance, maintaining over 90 % NO x conversion even in the presence of SO 2 and H 2 O. Our work opens a new avenue for developing low-temperature NH 3 -SCR catalysts with desired SO 2 and H 2 O resistance, offering valuable insights for advancing catalytic performance in challenging reaction conditions.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2024
·
IF 2
Jie Li,Huan Zhou,Jie Yang,Cunbing Xu,Sifan Wang,Yifan Li,Jiangbo Chen
The solid–liquid phase equilibria of the Li+, Na+, Ca2+//Cl––H2O quaternary system at 298.15 and 323.15 K are studied via the isothermal solubility phase equilibrium method. The solubility data and liquid properties of density and pH are obtained. The phase diagrams of the quaternary systems, including the water free diagram, the water diagram, and the dry salt diagram, are plotted to show the phase regions, water content, and salting-in effect. NaCl occupies the largest phase region at both 298.15 and 323.15 K. One double salt LiCl·CaCl2·5H2O occurs at 298.15 K and builds up two invariant points; one incommensurate invariant point saturated by (NaCl, LiCl·H2O, LiCl·CaCl2·5H2O) and one commensurate invariant point saturated by (NaCl, CaCl2·4H2O, LiCl·CaCl2·5H2O), but at 323.15 K, no double salt forms. The salting-in effect that happened in ternary systems still occurs in the quaternary Li+, Na+, Ca2+// Cl––H2O system at both temperatures. NaCl saturated concentration increases with LiCl and CaCl2 contents and results in a very high total salt content at commensurate invariant points, e.g., they are 56.92 and 60.62% at 298.15 and 323.15 K, respectively.
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Small
·
2025
·
IF 12.1
Xiang Liu,Yongxin Fu,Ruidong Li,Yurong Yin,Jun Hu,Binran Zhao,Chengyi Dai,Xiaoxun Ma,Chunshan Song
Directly converting methane into high-value-added chemicals presents a significant challenge in catalysis. Nonthermal plasma (NTP) offers an efficient approach for direct methanol synthesis through methane activation. However, theoretical frameworks for designing catalysts under NTP conditions remain underdeveloped. It is quite difficult to control the assembly process of radical species on catalyst surfaces. A boron nitride (BN)-confined Fe single-atom catalysts (Fe-SACs) is synthesized by in situ anchoring in defect sites induced by mechanical ball milling. This catalyst is utilized for NTP-catalyzed direct methane-to-methanol conversion. The results demonstrate that the CH 3 OH yield increases by ≈2.5 times compared to conditions with NTP alone, while selectivity doubles. The experimental results and theoretical calculations indicate that ·OH radicals generated by the dissociation of H 2 O are rapidly adsorbed by Fe-SACs before annihilation. This process facilitates the stabilization of ·CH 3 species and enhances the kinetics of CH 3 OH assembly along the E-R reaction pathway. A design criterion is proposed for plasma-catalyzed radical adsorption intensification-directed assembly catalysts, offering a novel approach for the directional catalytic conversion of reactants through radical pathways.
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高影响因子
Sustainable Energy & Fuels
·
2018
·Vol. 2
·期 7
·1481-1490
·
IF 0
Rong Zhou,Jianxing Huang,Shaobo Lai,Jiyang Li,Feng Wang,Zhiqiang Chen,Weiqing Lin,Chao Li,Jing Wang,Jinbao Zhao
A novel strategy for selecting an additive based on understanding the influence of different functional groups on electrochemical characteristics is adopted. N,N-Diethylamino trimethylsilane (DEATMS) is tested as a bifunctional electrolyte additive to scavenge H2O and neutralize HF in the electrolyte and enhance the behaviour of graphite/LiNi0.5Co0.2Mn0.3O2 cells operating at a high voltage (4.5 V vs. Li/Li+) or elevated temperature (55 °C). With 2% DEATMS, no LiPF6 hydrolysis species is found after storage at 55 °C for 6 days, even with a moisture content of 2000 ppm in the electrolyte. In addition, the graphite/LiNi0.5Co0.2Mn0.3O2 cells containing DEATMS show cycling performances superior to those of the cells without DEATMS upon cycling for 100 cycles at a high voltage (85.5% vs. 72.0%) or high temperature (81.2% vs. 70.6%). The sacrificial oxidation of DEATMS on the cathode surface restricts direct contact between the electrolyte and cathode, improving the electrochemical performance. The ex situ surface analysis of the electrodes after cycling indicates that both the electrolyte decomposition and Mn dissolution are inhibited by the deposition of DEATMS oxidation products.
研究领域:
材料科学
·
电化学
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Catalysis Science & Technology
·
2025
·
IF 4.2
Junjie Jiang,Yang Zou,Xue Li,Yongqi Zhao,Ziwei Zhao,Xiaolong Liu,Tingyu Zhu
Noble metal catalysts exhibit high efficiency and stability in CO removal, but their high loading of noble metals led to elevated costs, limiting industrial applications. This study selected three representative noble metals (Pt, Au, Ru) to investigate the CO reaction mechanisms on low-loading noble metal catalysts and the effects of SO2/H2O on CO oxidation. Catalysts with 0.1 wt% metal loading were synthesized via the impregnation method using conventional TiO2 as the support, denoted as 0.1Pt/Ti, 0.1Au/Ti and 0.1Ru/Ti. Among them, 0.1Pt/Ti achieved complete CO conversion at 270 °C and maintained 100% conversion over 46 h of continuous operation at 250 °C in the presence of SO2 and H2O. In situ DRIFTS indicated that the CO reaction over all catalysts followed the Mars–van Krevelen (MvK) mechanism. However, both Langmuir–Hinshelwood (L–H) and MvK pathways coexisted on 0.1Pt/Ti, with the L–H mechanism being dominant. DFT calculations revealed that CO also exhibited a higher adsorption preference for the 0.1Pt/Ti catalyst, which was identified as the primary reason for its superior performance.
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