Journal of Magnesium and Alloys
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2025
·
IF 13.8
Zexuan Yang,Yazhou Wang,Xia Lin,Yongjin Zou,Cuili Xiang,Fen Xu,Lixian Sun,Yong Shen Chua
Magnesium-based hydrogen storage materials, such as MgH 2 , have attracted considerable attention because of its superior hydrogen storage capacities, inexpensive, and excellent reversibility. However, their high thermodynamic stabilities and slow kinetics lead to relatively high desorption temperatures, which severely limit the wide application of MgH 2 . In this study, the inclusion of vanadium induced the formation Ni-Co metal–organic frameworks (MOF) from a NiCo layered double hydroxide (LDH), thereby increasing the number of defects and vacancies, and improving the hydrogen storage properties of MgH 2 . The synthesized NiCo-MOF/V-O-doped MgH 2 system demonstrates excellent hydrogen storage capacity. More specifically, 5 wt.% of H 2 was released over 20 min at a relatively low dehydrogenation temperature of 250 °C, and almost complete dehydrogenation was achieved at 300 °C for 5 min. In addition, at 125 °C, the hydrogen storage material absorbed 5.5 wt.% H 2 in 10 min. Furthermore, the activation energy of dehydrogenation was determined to be 69.588 ± 6.302 kJ ·mol −1 which is significantly lower than that of the ball-milled MgH 2 (i.e., 118.649 ± 2.825 kJ ·mol −1 ). It was therefore inferred that during dehydrogenation process, a Mg 2 Ni/Mg 2 NiH 4 hydrogen pump is formed by Ni, while the V-H and Co-H bonds formed by Co and V during the reaction act synergistically to catalyze the absorption and desorption of hydrogen, thereby increasing the hydrogen storage capacity of MgH 2 . These experiments provide new perspectives on the commercial application of MgH 2 .
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Linsen Li,Zhuwei Yang,Xiao Yang,Hui Xiong,Zhao Jiang,Tao Fang
Liquid organic hydrogen carriers (LOHCs) are considered as promising candidates for large-scale hydrogen storage, which offers significant advantages in terms of hydrogen storage density, ease of storage and transportation. NPhCZ (N-phenylcarbazole)/18H-NPhCZ (perhydro-N-phenylcarbazole) is proposed as a typical system with high hydrogen storage capacity. However, low dehydrogenation activity and selectivity of catalysts restrict the cyclic efficiency of hydrogen storage. In this study, the efficient catalysts are designed by the immobilization of ultrafine, highly dispersed Pd nanoparticles onto Ni, N co-doped carbon materials through wet chemical reduction. The Pd/Ni@NC-10 catalyst exhibits the highest catalytic performance with 100 % conversion, 81.9 % selectivity of NPhCZ and 6.48 wt% hydrogen release amount. Combined with XRD, HRTEM, Raman, XPS, H 2 -TPR, N 2 physisorption characterization methods and DFT calculations, it is found that the doped Ni, N species could synergistically increase the dispersion of loaded Pd nanoparticles, as well as regulate the electronic state around Pd, which in turn accelerates the rate of the rate-limiting step. The evident interaction between Pd nanoparticles and Ni, N co-doped carbon brings the enhancement of dehydrogenation efficiency. Besides, the spent catalysts are measured by XRD, TEM, XPS and evaluated for the dehydrogenation reaction, indicating that Pd/Ni@NC-10 shows good structural stability, durability and recyclability. It provides practical guidance for the design of LOHCs dehydrogenation catalysts.
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CHEMICAL ENGINEERING JOURNAL
·
2024
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IF 13.3
Huimin Li,Zhe Sun,Chenlong Dong,Xueli Zhang,Chengkun Lei,Baobao Jin,Qianqian Shen,Husheng Jia,Jinbo Xue
Photocatalytic non-oxidative coupling of methane is an attractive strategy for CH 4 to C 2 conversion, how to facilitate the photogenerated charge separation and accelerate the C–C coupling to promote the reaction kinetics remains a great challenge. Herein, a symbiotic r-Fe 2 O 3 /NiO heterostructure with robust interfaces is constructed in situ. The coherent interface not only provides unique Ni–O–Fe asymmetric sites, but also achieves the separation and transport of photogenerated charge. The unbalanced charge density distribution of two adjacent methyl or methylene at the Ni–O–Fe asymmetric site alleviates the dipole repulsion of the C–C coupling, and promotes C–C coupling to form C 2 hydrocarbons. Under visible light irradiation, the optimal r-Fe 2 O 3 /NiO performs a brilliant C 2 activity up to 71.00 μmol g −1 h −1 , and the C 2 H 4 yield can reach a high value of 40.46 μmol g −1 h −1 and the selectivity of 56.98 %. This work provides new insights into the coupling of C–C to generate C 2 hydrocarbons.
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JOURNAL OF CATALYSIS
·
2024
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IF 6.5
Yixuan Wang,Hongyan Ban,Yugao Wang,Ruwei Yao,Shimin Zhao,Jiangliang Hu,Congming Li
Basic sites profoundly affect the mode and strength of CO 2 adsorption in the hydrogenation of CO 2 to formic acid (FA), however, the mechanism by which the quantities and strength of basic sites affect the reaction process is not yet clear. Herein, a Ni/Mg a AlO x catalyst has been developed and the basic sites of the catalyst can be modulated by simply altering the Mg/Al ratio. Through a series of characterizations and experiments, it was observed that weak and medium basic sites synergistically catalyzed the hydrogenation of CO 2 to formic acid, and a reasonable number of weak basic sites can improve reaction performance when a sufficient number of medium basic sites guarantee the fundamental catalytic activity. Moreover, the number and distribution of basic sites are also tightly related to metal-support interactions. This strategy provides theoretical guidance and a feasible scheme for optimizing the performance of non-precious metal heterogeneous catalysts.
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Surfaces and Interfaces
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2024
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IF 5.7
Xuanqi Hao,Wenbin Shi,Ping Yang
To address the issues of low photoluminescence quantum yields (PLQYs), broad PL spectra, and poor stability, multicolor carbon dots (CDs) were synthesized by using different precursors. Blue-emitting CDs were created via a solvothermal synthesis by using citric acid and ethylenediamine while green-emitting CDs were fabricated using O-phenylenediamine. Ni doping further increased the PLQYs and stability of CDs. Ni-doped CDs (Ni-CDs) with blue- and green-emitting were synthesized through a one-step solvothermal method. The PL peak wavelengths of Ni-doped blue CDs (Ni-BCDs) and Ni-doped green CDs (Ni-GCDs) were located at 450 and 540 nm, respectively. After Ni-doping, the average particle size of green-emitting CDs was increased from 2.35 to 2.65 nm. Compared with undoped CDs, Ni-CDs exhibited narrow PL spectra, high PLQYs, and long fluorescent lifetime. The PLQYs of Ni-BCDs and Ni-GCDs were increased to 83.92 and 35.60 %, respectively. Interestingly, the PL peak wavelengths of Ni-doped CDs revealed a red-shift with increasing the solvent polarity (e.g. acetone, acetonitrile , N, N-dimethylformamide, tetrahydrofuran, dimethyl sulfoxide , ethanol, methanol, and H 2 O). In addition, the PL peaks of green-emitting Ni-CDs generated a large red-shift with increase the ratio of water in organic solvents compared with blue one. Namely, solid Ni-GCDs powders also revealed water dependent PL. After incorporating the CDs in flexible films, Ni-GCDs still revealed high brightness and stability. These results supplied important possibility for the application of multicolor CDs.
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NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 36
·15870-15883
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IF 2.7
Chuhan Xing,Yaoyao Chen,Zhi Song,Boxia Liu,Xiayan Zhang,Jialu Liu,Yeqiong Huang,Dongxu Han
Norfloxacin (NOR) is a synthetic antibacterial agent that is extensively applied in the management of various infectious conditions. After entering the human body, most of it cannot be absorbed and is excreted, eventually reaching natural waters. At the same time, it promotes the generation of drug-resistant bacteria, which seriously threatens human health. In this study, a simple mechanical mixing method was employed to synthesize a Ni–MCM composite catalyst with excellent stability, which was utilized for the degradation of NOR. The effects of the mass ratio of Ni–MC to MCM-41, initial pH value, starting NOR concentration, catalyst dosage and inorganic anions on NOR degradation were studied. The findings indicate the superior degradation capability of Ni–MCM towards NOR under diverse conditions. Quenching experiment and electron paramagnetic resonance spectroscopy showed that when dissolved oxygen occupied the active site of the metal in the catalyst, more ˙O2− and 1O2 would be formed, and NOR would be degraded due to the interaction with the mixed system composed of ˙OH and SO4˙− and electron transfer, indicating that the degradation mechanism of the Ni–MCM system was dominated by non-free radicals. The utilization of the Ni–MCM nano-composite catalyst is a promising approach for the treatment of wastewater containing norfloxacin.
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RARE METALS
·
2025
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IF 11
Zhi Song-Song,Zou Xiao-Xiao,Lei Jin-Ye,Zhang Lu,Li Zi-Han,Gu Wan-Nuo,Ullah Fahim,Guo Hong,Wu Da-Peng
Photocatalytic CO 2 reduction using atomically dispersed catalysts holds significant potential for addressing global energy and environmental challenges. However, the influence of d–d orbital interactions between metal centers and coordinated atoms remains underexplored. Herein, nickel phthalocyanine is anchored to the metal-exposed crystal face of TiO 2 , forming Ti–Ni–N 4 coordination. This configuration reveals that the axially coordinated Ti atoms serve as a novel electron channel with electron-donating ability, transferring electrons to the Ni center through d–d coupling. It is found that the dynamic adjustment of bond lengths and d-band centers in Ti–Ni bonding during CO 2 photoreduction process can effectively modulate the adsorption strengths of the Ni center for different intermediates. This leads to a significant enhancement in the photocatalytic performance for CO 2 reduction to CO without a sacrificial reagent, achieving an exceptional CO evolution rate of 378.5 μmol g −1 . Furthermore, the d–d coupling mediated by Ti–Ni–N 4 coordination increases the vacancy formation energy of active sites, preventing the leaching of Ni active centers. This study provides a strategy for the precise design of d–d orbital regulation and resistance to demetallization in photocatalysts for efficient CO 2 conversion. Graphic abstract
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2025
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IF 8.3
Jie Jiang,Zhenzhen Xue,Yawei Wang,Di Tang,Rongfeng Yuan,Ning Ma,Alaa S. Abd-El-Aziz
12H-NECZ (dodecahydro-N-ethylcarbazole), a promising liquid organic hydrogen carrier (LOHC) with high H 2 capacity, stability, and low dehydrogenation temperature, requires efficient low-cost dehydrogenation catalysts for industrial-scale application. In this work, NiCuAl-LDH-R (hydrotalcite-derived NiCu bimetallic catalyst) with rosette-like two-dimensional structures and highly dispersed NiCu alloys are prepared for the dehydrogenation reaction of 12H-NECZ. The addition of Cu to NiAl-LDH-R can significantly reduce the reaction temperature while achieving rapid dehydrogenation. Among the NiCuAl-LDH-R catalysts, the Ni 7 CuAl-LDH-R exhibited the highest dehydrogenation performance with 100 % dehydrogenation efficiency and 100 % selectivity of NECZ at 180 °C within 4h (12H-NECZ/catalyst mass ratio = 15:1). The electronic and geometric effects of Ni and Cu, excellent dispersion of NiCu alloy, strong metal carrier interaction between NiCu alloy and AlOx, as well as the rich alkalinity synergistically contributes to the catalyst's exceptional dehydrogenation activity. The cost-effective nonprecious catalyst, with tunable morphology/composition and excellent performance, shows great potential for 12H-NECZ dehydrogenation applications.
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SENSORS AND ACTUATORS B-CHEMICAL
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2025
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IF 7.7
Lingnan Kong,Quanhua Xie,Yuanyuan He,Shiyu Dong,Yang Liu,Wenliang Fan,Haiyan Yao,Mingfu Zhao,Nianbing Zhong
This paper proposes a polyvinyl alcohol/AlFFIVE-1-Ni (PVA/KAUST-8)-coated long-period fiber grating (LPFG) SO 2 concentration sensor to accurately monitor SO 2 concentrations online. To enhance the adhesion strength between the fiber and a SO 2 -sensitive film, the etched LPFG surface was silanized using 3-aminopropyltriethoxysilane, and then coated with a PVA/KAUST-8 SO 2 -sensitive sol using the doctor blading method. A fluorosilane hydrophobic coating was deposited on the SO 2 -sensitive membrane surface and integrated with a LPFG temperature sensor, thereby effectively eliminating measurement interference caused by ambient temperature and humidity fluctuations during SO 2 concentration detection. The morphology and composition of the SO 2 -sensitive films were characterized using optical microscopy, field-emission scanning electron microscopy, X-ray diffraction analysis, and X-ray photoelectron spectroscopy. Furthermore, the working principle of the sensors for the detection of SO 2 was established. Under optimized parameters (LPFG diameter: 60 μm; PVA doping in PVA/KAUST-8: 12 wt%; SO 2 -sensitive film: 45 μm; fluorosilane composite layers: 12) within a humidity range of 0–60 % RH and a temperature range of 25–45 °C, the sensor demonstrated a good selective SO 2 detection with 2.79 pm/ppm sensitivity, 1.07 ppm detection limit, 390 s response time, and 8.89 % maximum relative error.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2025
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IF 21.1
Ziwei Ma,Jingyi Wang,Wei Wang,Xueyi Song,Yating Liu,Shaobin Wang,Yunjin Yao
We engineered a NiSe/Ni₃Se₂ heterostructure on nickel foam that activates formic acid for rapid hexavalent chromium detoxification. We used one-step hydrothermal growth and probed structure and mechanism by diffraction and spectroscopy, electron microscopy, electron paramagnetic resonance with 5,5-dimethyl-1-pyrroline N-oxide, and batch and fixed-bed tests. The optimized catalyst removed 99.7% of 50 mg L⁻¹ hexavalent chromium in 40 minutes at 25 °C, achieved full removal of 1 mg L⁻¹ in 20 minutes, tolerated common ions, and maintained 100% removal for 180 h in continuous flow. Mechanistic analyses show a radical pathway dominated by hydrogen radicals (H ⁎ ) and carbon dioxide radical anions ( C O 2 • − ), promoted by selenium vacancies and tightly coupled nickel selenide interfaces that accelerate formic-acid activation and interfacial charge transfer. Operating without external energy input, this monolithic architecture avoids powder recovery and minimizes pressure drop and cost, offering a general route to defect-engineered selenides for efficient, low-cost environmental redox remediation.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Ziyang Xu,Liang Chen,Zeyu Liu,Jiaying Xing,Edward J. Anthony,Chunbo Wang
Methanol synthesis from CO 2 hydrogenation is a promising route for carbon–neutral fuel production, but conventional Cu-based catalysts suffer from poor activity at low pressure. Herein, we report a cost-effective and scalable dual-site Ni n /Cu 1 -A catalyst, designed by integrating Ni nanoparticles (NPs) with Cu single atoms (SAs), for CO 2 hydrogenation to methanol at ambient pressure. The obtained Ni n /Cu 1 -A catalyst achieves a remarkable methanol STY of 665.7 μmol g cat -1 h −1 at 240 °C and 0.1 MPa, significantly outperforming both monometallic Cu 1 -A (199.7 μmol g cat -1 h −1 ) and Ni n -A (38.4 μmol g cat -1 h −1 ) catalysts. Further investigations reveal that Ni NPs facilitate hydrogen activation and spillover, while Cu SAs serve as the primary active sites for CO 2 reduction to methanol, effectively promoting the formate-mediated reaction pathway. This synergistic interaction leads to a substantial enhancement in CO 2 -to-methanol conversion. This work develops an efficient catalyst for CO 2 hydrogenation under mild conditions and provides a promising strategy for distributed green methanol synthesis in small-scale systems, enabling sustainable CO 2 utilization through renewable energy integration.
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Reaction Chemistry & Engineering
·
2025
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IF 3.1
Zihao Bu,Kuo Zhou,Jialin Xu,Yuhao Wu,Shengrong Guo
The sustainable production of carbamates from biomass-derived molecules provides a viable alternative to petrochemical-based production routes. In this work, we reported an efficient catalytic strategy for synthesizing bio-based furfurylmethyl carbamate (FMC) through methoxycarbonylation of furfurylamine with dimethyl carbonate (DMC) under mild conditions. A novel Pb-Ni composite oxide catalyst with high activity and stability was developed, which significantly outperformed conventional monometallic oxide catalysts. Comprehensive characterization revealed that the synergistic interaction between Pb and Ni species constructed composite oxide nanoparticles (about 11.4 nm), with Pb species highly dispersed on the NiO matrix. Consequently, highly defective structure, abundant acid-base dual sites, and a high specific surface area were concurrently formed, which were identified as critical factors for activating both nucleophilic and electrophilic reactants. Significantly, appreciable quantities of furfuryl isocyanate were detected, demonstrating the feasibility of a one-pot cascade synthesis of bio-based isocyanates from amines and DMC.
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