FUEL PROCESSING TECHNOLOGY
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2023
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IF 7.5
Qiang Le,Zan Liu,Zhilin Cheng
In this work, a novel core-shell nanostructured coaxial nanofiber membranes (CFMs) were successfully produced by the coaxial electrospinning . The structure and composition of CFMs were probed by a series of characterizations. The results demonstrated that the CFMs were comprised of the versatile core-shell structure nanofibers, therein Cu(I)/UIO-66 scattered in the shell layer and HNTs dispersed in the core layer. As applied in the selective adsorption desulfurization , the Cu(I)/UIO-66 embedded on the surface of the nanofiber undertook the adsorption active sites, while HNTs in core layer served as enhancing the mechanical performance of PAN nanofibers. The CFMs had the superior adsorption performance in the batch adsorption (maximum:40.14 mg·g −1 ) and fixed-bed adsorption (maximum: 47.43 mg·g −1 ) capacities for benzothiophene (BT) from fuel oil, respectively. Furthermore, due to having the robust mechanical performance, the CFMs exhibited the preferable recycling adsorption and mechanical stability . The adsorption mechanism of BT molecules on CFMs was explored by the kinetics, isotherms and thermodynamic models , indicating the existence of the synergistic effect of physical adsorption and chemical adsorption.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Jiaxian Liu,Guyang Ning,Kun Shi,Man Zheng,Yuena Sun,Yongjun Gao,Yufan Zhang,Huan Wang
In this work, a string of different proportion trimetallic loaded the N-doped hollow porous carbon nanospheres (N-HPCS@Co Cu Fe NSs) were successfully crafted by a simple and economical method. Herein, the hollow-carbon structure was formed by etching carbon nanospheres. Moreover, owing to the presence of the PDA and P123, high dispersed nano spheres with mesopores were obtained. By this way, the catalyst can expose unique internal cavity and short transport path. Meanwhile, trimetal-based metal-organic frameworks (MOFs) Co Cu Fe alloy nano spheres (Co Cu Fe NSs) are first prepared. Creatively, PDA acts as the carbon resource, nitrogen resource and metal grafting agent simultaneously. Through a series of tests, N-HPCS@Co 1 Cu 1 Fe NSs has the best electrocatalytic performance and durable stability. This work highlights the current advances of hollow porous carbon structure, trimetallic active sites and N-doping, as well as, endow high electrocatalytic activity and durability for HER and OER .
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DALTON TRANSACTIONS
·
2021
·Vol. 51
·期 3
·904-909
·
IF 4.39
Chang Liu,He-Di Yang,Pei-Pei Hou,Yu Xiao,Yi Liu,Hua Lin
Inorganic chalcogenides containing cations with lone-pair electrons have attracted considerable attention because of their potential applications in photocatalysis. In this research, two new copper thioarsenates with the lowest Cu-to-As ratio in the quaternary X/Cu/As/Q (X = inorganic cations; Q = chalcogen) system, namely Cs3CuAs4Q8 (Q = S, Se), were obtained by a simple surfactant–thermal method at a low temperature. These two isostructural compounds belong to the monoclinic space group C2/c (no. 15) and are composed charge-balanced Cs+ cations and two-dimensional anionic [CuAs4Q8]3− layers. Notably, photo-electrochemical measurements indicate that Cs3CuAs4Q8 possesses a remarkable photocurrent response under simulated solar-light illumination. Further theoretical studies were performed to gain insights into the relationships between electronic structure and optical properties.
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PubMed
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ACS Applied Nano Materials
·
2023
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IF 5.9
Zhaolei Ma,Ruoning Bai,Wei Yu,Guoxian Li,Chuizhou Meng
Transition metal single atoms have been considered as promising candidates for oxygen reduction reaction catalysts for developing high-performance zinc–air batteries. How to uniformly disperse metal single atoms onto an ideal porous carbon framework for full utilization of the catalyst with enriched active sites and fast mass diffusion still remains a challenge. Herein, by taking advantage of both the efficient single-atom Cu catalyst and the effective NaCl-template sacrificing method, we report the design and fabrication of a single-atom Cu catalyst decorated on a three-dimensional (3D) nitrogen–carbon (NC) framework. The developed catalyst exhibits excellent (oxygen reduction reaction) ORR catalytic activity with a high half-wave potential of 0.86 V, maximum current density of 5.53 mA cm–2, and Tafel slope of 81.52 mV dec–1, which are better than those of the commercial Pt/C catalyst. The comparison experiment with the 3D NC framework (no copper salt added) and the bulk Cu decorated NC framework (no NaCl added) verifies the synergistic effect between the Cu single atoms as the efficient ORR catalyst and the NaCl template to achieve the ideal porous structure. Aqueous zinc–air batteries assembled with the developed catalyst deliver good battery performance with a high open circuit voltage of 1.48 V, large specific discharge capacity of 760.47 mAh g–1, high peak power density of 120 mW cm–2, and stable charge–discharge cyclability for 600 h. Gel polymer electrolyte-based zinc–air batteries are also demonstrated to be workable under bending conditions for practical wearable electronic applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Yaoyao Zhang,Shikui Jia,Xinqiang Yuan,Liu Ding,Taotao Ai,Kangze Yuan,Wei Wang,Luca Magagnin,Zhenyi Jiang
In this work, a novel adsorbent was evaluated for eliminating heavy metal ions from water. The cyano-functionalized silica aerogels (ANSA-X) were fabricated by functionalizing silica aerogel with 2-cyanoethyltriethoxysilane, and then further by the reaction with hydroxylamine hydrochloride to obtain amidoxime-functionalized silica aerogels (AOSA-X) with a large specific surface area. The FTIR and NMR analysis indicated that cyano was successfully transformed into amidoxime groups. Adsorption experiments showed the adsorption performed well with the Langmuir isotherm, and AOSA3 exhibited the optimum adsorption property with 598.05 mg/g for Pb (II) and 534.10 mg/g for Cu (II). The thermodynamic results indicated that spontaneous endothermic process was the nature of the adsorption. The adsorption rate of AOSA3 was above 86% after five successive adsorption–desorption cycles. XPS analysis and DFT calculations demonstrated that the N and O atoms participated in the chelating adsorption of Pb (II) and Cu (II), and the N atom on the amidoxime groups played a dominant role. Life Cycle Analysis (LCA) evaluated the environmental effect of the preparation of 1 kg AOSA3 adsorbent, identified the environmental factors with high environmental impact, proposed alternative solutions, proved the feasibility of preparing a novel high-efficiency amidoxime-based adsorbent, and provided a guideline for the sustainable mass production of AOSA3 adsorbent. In conclusion, AOSA3 demonstrated to have promising application perspectives in heavy metal effluent treatment.
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CERAMICS INTERNATIONAL
·
2023
·
IF 5.2
Xinfei Zhang,Panpan Lin,Jincheng Lin,Xinyue Li,Shuye Zhang,Fugang Lu,Zihan Cong,Ce Wang,Peng He,Tiesong Lin
A novel transient liquid phase bonding (TLP) method for obtaining high-temperature resistant diamond/Cu joint was designed. The joint was achieved through the isothermal solidification of Au–Si interlayer assisted by the diamond active modified layer and NiTi particles. The interfacial reaction mechanisms in the TLP process were systematically investigated in this study. The results shown that Ti 5 Si 3 C, CuTiSi and NiTiSi precipitated from the seam. Due to the precipitation of Si and the interdiffusion of Au–Cu, a ductile Au–Cu solid solution ((Au, Cu)ss) matrix formed. The shear strength of the diamond/Cu joint was notably affected by the holding time. The maximum room-temperature shear strength of 108 MPa was achieved when the joints were held at 600 °C for 60 min, and the high-temperature strength was still up to 22 MPa at 600 °C. The high strength of the joints was achieved because of (i) the elimination of the Cu(Au)–Si brittle phases, (ii) the NiTiSi whiskers pulling-out mechanism, and (iii) the moderate distribution of compounds at the diamond/seam interface.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Linzhi Shen,Ziwen Xiong,Zhaohui Du,Hao Wang,Wenrui Li,Zhen Zhang,Hao Wu,Changsong Zhou,Yaming Zhou,Guanghua Tang,Jing Liu,Hongmin Yang
M-N-C catalysts have considerable potential in the fields of catalysis, such as highly polluting gaseous elemental mercury (Hg 0 ) oxidation. However, the direct application of these kinds of catalysts for mercury removal is stymied by their low catalytic efficiency. Heteroatom-doping in M-N-C catalysts has been proposed as a powerful strategy to the promote catalytic of Hg 0 , but the origin of boosting catalytic activity is still elusive. Herein, it is disclosed that selenium doping induces an obvious electron-acceptor effect for accelerating the Hg 0 catalytic oxidation. The model selenium-doped Cu-N-C catalyst with atomically dispersed active sites was verified by various characterization methods, such as SEM-EDS and scanning transmission electron microscopy. The optimal Cu-NC-Se with Cu/Se ratio of 1:1 exhibited the best Hg 0 removal performance, over 8-fold enhancement in their Hg 0 oxidation capacities than raw selenium-free Cu-NC. At the optimal reaction temperature of 90 °C, Cu-NC-Se achieved an average Hg 0 removal rate of 92.44% within 60 min under single pure N 2 atmosphere. As for the influence of flue gas components, the presence of O 2 promoted the removal of mercury in Cu-NC-Se, whereas CO 2 , NO and SO 2 served as slight inhibitors. Even after five cycles of the experiment, the average mercury oxidization efficiency was still remained at 88.5%, showing that Cu-NC-Se can be reused with good maintenance of the catalytic activity and atomic dispersion of Cu and Se in the structure. The unsaturated Cu sites connected with pyridinic N on the carbon matrix can serve preferential adsorption to Hg 0 and doped selenium. Meanwhile, the selenium doping accelerated Hg 0 adsorption and accept sufficient electrons for promoting Hg 0 oxidation to forming stable HgSe, which is also corroborated by the theoretical analysis results based on density functional theory. This work not only provides an alternative facile synthetic strategy for developing heteroatom-doping atomically dispersed M-N-C catalysts, but also represents a significant advance for deepening the understanding of the Hg 0 catalytic oxidation mechanism on M-N-C catalyst.
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INORGANICA CHIMICA ACTA
·
2023
·
IF 2.8
Qiu Lv,Qing Lin Guan,Xiao Yu Tang,Jing Jin,Feng Ying Bai,Yong Heng Xing
Nitrogen heterocyclic polycarboxylic acid is a type of ligands with excellent coordination ability and rich conformations. Two metal complexes, ([Co 2 (L 1 ) 2 (CH 3 COO)(H 2 O) 3 ]‧(CH 3 COO)‧H 2 O ( 1 ) (HL 1 = 4-[2,6-bis(pyrazin-2-yl) pyrid-4-yl]benzoic acid)) and (Cu 2 (L 2 )(H 2 O) ( 2 ) (H 4 L 2 = 5-[6-(3,5-dicarboxy phenylamino)pyrid-2-ylamino]benzene-1,3-dicarboxylic acid)) were synthesized with transition metal salts and nitrogen heterocycle polycarboxylic acid ligands by solvothermal method. Both complexes were characterized by infrared and ultraviolet spectroscopy, powder X-ray diffraction analysis, and thermogravimetric analysis. The X-ray single crystal structural analysis shows that complex 1 is a one-dimensional double-chain supramolecular structure built by intermolecular hydrogen bonds. While complex 2 is a three-dimensional framework with multiple channels, where the two independent Cu(II) metals are five-coordinated to form a square pyramidal coordination geometry. In addition, in order to investigate the functional properties of the two complexes, catalytic reduction experiments towards p-nitrophenol were carried out preliminarily. The reduction efficiency above 96 % demonstrates their potential as catalysts.
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NEW CARBON MATERIALS
·
2026
·Vol. 41
·期 4
·1054-1067
·
IF 7.2
Sheng Wang,Zhijia Chen,Xiao Wang,Chunhua Yuan,Songbo Li,Huimin Yang
Adipic acid is widely used in fine chemical synthesis, biomedicine and other industrial fields, and is a key monomer for the synthesis of nylon-6,6 and nylon-6. Industrially, it is produced by the efficient catalytic oxidation of cyclohexane. However, the activation of the inert C―H bonds in cyclohexane remains a major challenge in the highly selective synthesis of acid products. Using a composite catalyst of copper on a carbon support produced from wood chip biomass, a green catalytic system was established for the one-pot oxidative synthesis of adipic acid from cyclohexane. Wood chips has two functions during pyrolysis: it acts as a carbon support precursor and an in-situ reducing agent, which reduces Cu 2+ into Cu/Cu 2 O active species to obtain Cu/Cu 2 O@C composite catalysts. The abundant defects in biomass carbon form strong coordination interactions with the copper active components, which effectively regulate the electronic distribution of active sites and improve the catalytic performance. Under optimized conditions (100 °C, 12 h), the Cu/Cu 2 O@C-0.1 catalyst achieves a cyclohexane conversion of 19.36% and an adipic acid selectivity of 73.28%. Mechanistic investigations show that the electronic interaction between the biomass carbon support and the copper species strengthens the adsorption of cyclohexanone, which is critical for promoting the selective formation of adipic acid. This study provides a viable strategy for developing eco-friendly, low-cost and high-efficiency advanced catalytic materials. Download: Download high-res image (138KB) Download: Download full-size image
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 24
·10530-10537
·
IF 9.8
Jiangang Yu,Pingnian Bao,Jia Liu,Yi Jin,Jie Li,Yanwen Lv
In this study, cellulose nanofibrils (CNF) and transition metals (Cu and Ni) were used as the matrix and doping agents, respectively, for the controllable synthesis of ZnO@CNF nanocomposites with adjustable visible-light photocatalytic properties. All samples were elaborately characterized by Fourier transform infrared spectroscopy, Brunauer–Emmett–Teller, X-ray diffraction, scanning electron microscopy-energy dispersive spectrometry, X-ray photoelectron spectroscopy, UV-Vis diffuse reflectance and photocurrent response. Several nano-ZnO particle morphologies, including plate, nanorod, sphere, and star, were produced and anchored on the CNFs by controlling the ZnO loading ratio. The as-produced ZnO@CNF nanocomposites exhibited a remarkable photocatalytic degradation of methyl orange under visible-light irradiation. The plate-like ZnO0.6@CNF exhibited the best photodegradation efficiency (53.1%) for methyl orange under blue light (λmax = 450 nm, 50 W) irradiation. Furthermore, when doped with transition metals, Cu or/and Ni–ZnO0.6@CNF exhibited better photocatalytic efficiency than pristine ZnO0.6@CNF. Under blue light irradiation, the preferred Cu/Ni–ZnO0.6@CNF nanocomposite sample demonstrated an enhanced degradation efficiency for various wastewater pollutants, including methyl orange (96.6%), tetracycline hydrochloride (96.6%), rhodamine B (99.0%), 4-nitrophenol (94.7%), bromocresol green (92.9%), bromothymol blue (88.3%), methylene blue (87.7%), 2-chlorophenol (27.5%), and aniline (19.5%), with the recyclability of more than ten times. This study provides new insights into the regulation of ZnO morphology for synthesizing efficient ZnO@CNF photocatalysts for wastewater pollutant degradation under visible-light irradiation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xueqin Wang,Tiesen Li,Chan Wang,Qingyan Cui,Tinghai Wang,Xiaojun Bao,Yuanyuan Yue
Designing a cost-effective and fast fabrication Cu-SSZ-13 with improved selective catalytic reduction of NO by ammonia (NH 3 -SCR) performance remains an open question. Here we report that LaCe-SSZ-13 zeolites were synthesized from spent fluid catalytic cracking catalyst within 12 h. After ion-exchanging with CuSO 4 solution, the obtained LaCeCu-SSZ-13 catalysts exhibit significantly higher catalytic activity and hydrothermal stability than conventional Cu-SSZ-13. Various characterizations reveal that La and Ce modification not only facilitates the disperse of isolated Cu 2+ species, but also effectively mitigates dealumination and inhibits copper species aggregation after hydrothermal aging. In-situ diffuse reflection infrared Fourier transform spectrum analyses demonstrate that La and Ce modification can accelerate the adsorption capacity for NH 3 and NO x and promote the decomposition of NH 4 NO 3 intermediate species on the catalyst, benefiting the improvement of low-temperature activity. The combination of experiments and theoretical calculations further demonstrate that the most stable positions of La and Ce are on different eight-membered rings in SSZ-13, and then Cu 2+ ions tend to enter eight-membered rings to enhance the NH 3 adsorption capacity and decrease the H 2 O adsorption capacity, which results in higher low-temperature activity and hydrothermal stability than Cu-SSZ-13. Our work provides a feasible strategy for preparing the efficient rare-earth-modified Cu-zeolite based NH 3 -SCR catalyst for nitrogen oxide abatement.
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EUROPEAN JOURNAL OF MEDICINAL CHEMISTRY
·
2021
·
IF 6.514
Wen-Ying Shen,Chun-Peng Jia,An-Na Mo,Hong Liang,Zhen-Feng Chen
Three Cu(II) complexes of quinoline derivatives as cancer chemodynamic therapy agents were synthesized and characterized. These complexes were heavily taken up by cells and reacted with cellular glutathione (GSH) to reduce Cu 2+ to Fenton-like Cu + , which catalyzed endogenous H 2 O 2 to produce the highly toxic hydroxyl radicals (•OH) to kill cancer cells. Cu1 and Cu2 initiated CAT activity declines, mitochondrial membrane potential and ATP concentration decrease, mitochondrial Ca 2+ overload and ER stress response, leading to cell cycle arrest in sub-G1 and cancer cell caspase-dependent apoptosis . On account of the high GSH and H 2 O 2 specific properties of the tumor microenvironment , Cu1 and Cu2 exhibited higher in vitro anticancer activity and lower toxicity to normal cells. Cu1 and Cu2 efficiently inhibited tumor growth in the SK-OV-3 xenograft mouse model without obvious systemic toxicity.
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