JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Wenpeng Hong,Yuhang Li,Haifeng Jiang,Yu Zhang,Wei Jia,Meng Song
Catalytic steam gasification is a promising route for converting plastic waste into valuable gaseous products. This work explores the heterogeneous catalytic gasification behavior of polystyrene (PS) in a two-stage fixed bed system, as well as the promotion mechanism for the generation of gaseous hydrocarbons. The obtained results indicate that adding MnCo 2 O 4 catalyst can effectively promote the formation of gaseous hydrocarbons. Further, the incorporation of Cu strengthens the above reaction process, resulting in a yield of 85.08 mmol/g for the C 1 -C 3 gaseous hydrocarbons. However, the doping of Ni has a negative effect on the generation of gaseous hydrocarbons. Moreover, an increase in the flow rate of steam within the system results in an initial rise followed by a decline in the yield of gaseous hydrocarbons. The optimal steam inflow is determined at 0.14 mL/min. The cycling test results of the catalyst show that the yield of the gaseous components of C 1 -C 3 can still be maintained at about 80 % of the initial state after five cycles. Finally, the synergistic pathway of steam and catalyst in PS gasification is elucidated. These works provide important and valuable guidance for the preparation of high-value gas-phase hydrocarbon products from waste plastics.
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CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Yongzhen Gao,Jingpeng Hu,Wen-Jing Yi,Jingyi Yang,Kai Jiang,Tao Yang,Zhihan Li,Meng Zhang,Zhongyi Liu,Benlai Wu
Support crystal phase plays a crucial role in the controlled C O hydrogenation over the supported catalysts. Herein, the effects of Al 2 O 3 crystal phase (α, θ, η, and γ) on the supported Cu-based catalyst is highlighted for furfural (FAL) hydrogenation to furfuryl alcohol (FA). The evaluation results show that Cu/η-Al 2 O 3 exhibits the best performance (FAL conversion: 99.7 %, FA selectivity: 94.0 %), highest TOF value (29.3 h −1 ) and lowest apparent activation energy (66.3 kJ/mol). The comprehensive characterizations unravel that Cu/η-Al 2 O 3 has the smallest Cu nanoparticles and the highest content of Cu + and Cu 0 , which facilitates H 2 dissociation and FAL adsorption. The reaction mechanisms suggest that Cu/η-Al 2 O 3 has the strongest FAL adsorption and FA desorption capacity. Moreover, it is demonstrated that FAL is linear chemical adsorption on the catalyst surface in the η 1 (O) configuration, which avoids the furan ring hydrogenation, and thereby, results in the high FA selectivity. This work would provide some references for developing the high-efficiency C O hydrogenation catalysts.
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Nanoscale
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2024
·Vol. 16
·期 22
·10727-10736
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IF 5.8
Peijiao Chen,Zhijun Li,Pengze Wang,Yuxin Yao,Tianwei Dou,Yang Qu,Liqiang Jing
The photocatalytic water-mediated CO2 reduction reaction, which holds great promise for the conversion of CO2 into valuable chemicals, is often hindered by inefficient separation of photogenerated charges and a lack of suitable catalytic sites. Herein, we have developed a glycerol coordination assembly approach to precisely control the distribution of atomically dispersed Cu species by occupying Ti-defects and adjusting the ratio between Cu species and Ti-defects in a hierarchical TiO2. The optimal sample demonstrates a ∼4-fold improvement in CO2-to-CO conversion compared to normal TiO2 nanoparticles. The high activity could be attributed to the Ti defects, which enhance the photogenerated charge separation and simultaneously facilitate the adsorption of water molecules, thereby promoting the water oxidation reaction. Moreover, by means of in situ EPR and FTIR spectra, we have demonstrated that Cu species can effectively capture photogenerated electrons and facilitate the adsorption of CO2, so as to catalyze the reduction of CO2. This work provides a strategy for the construction of atomic-level synergistic catalytic sites and the utilization of in situ techniques to reveal the underlying mechanism.
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CHEMICAL ENGINEERING JOURNAL
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2025
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IF 13.2
Shanguang Xu,Xin Han,Fan Zhang,Zhengyang Sun,Ruiying Chai,Fei Xu,Shanguo Du,Xiuling Jiao,Dairong Chen,Jie Zhang
The development of efficient catalysts for the selective hydrogenation of furfural (FAL) to furfuryl alcohol (FOL) is of great importance for sustainable chemical production. In this study, a highly efficient Cu/Al 2 O 3 catalyst was developed for the selective hydrogenation of FAL to FOL, achieving 100 % conversion and 100 % selectivity at 85 °C and 1.0 MPa H 2 with the optimal 7Cu/Al 2 O 3 -AIP catalyst, which was tailored by modulating the surface acidity of Al 2 O 3 and the distribution of Cu species. Evaluation of Cu-supported varying Al 2 O 3 catalysts revealed a near-linear correlation between the density of medium-strong acidic sites and catalytic activity, unequivocally demonstrating that medium-strong acidic sites on the alumina surface serve as the active sites for the reaction, which was further corroborated by competitive adsorption experiments involving pyridine and furfural. Furthermore, the density of Cu 0 sites was varied by adjusting the copper loading and conducting N 2 O selective oxidation experiments. Notably, a linear increase in catalytic activity was observed with the Cu 0 /(Cu 0 + Cu + ) ratio on the catalyst surface. Advanced characterization techniques, combined with experimental results, elucidated that the Cu 0 species act as the primary active sites for H 2 activation, while acidic sites are crucial for FAL adsorption, leading to the exceptional catalytic performance by the synergistic catalysis. This study underscores the synergistic effect between Cu 0 species and acidic sites, providing profound mechanistic insights into the FAL hydrogenation process and establishing a strategic foundation for the rational design of highly efficient Cu-based catalysts.
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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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CHINESE JOURNAL OF CATALYSIS
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2025
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IF 17.7
Bo Feng,Danning Feng,Yan Pei,Baoning Zong,Minghua Qiao,Wei Li
The photocatalytic oxidation of methane to methanol using molecule oxygen directly is an attractive catalytic reaction, but designing catalysts to avoid over-oxidation remains a significant challenge. Herein, Cu single-atom anchored on the defective carbon nitride structure (Cu SA/Def-CN) is designed for selective photocatalytic oxidation of methane into methanol using O 2 under mild conditions. The Cu SA/Def-CN catalyst exhibits a high methanol selectivity of 92.8% under optimized conditions. Mechanistic studies reveal a synergistic effect between Def-CN and Cu SA, where Def-CN is responsible for the in-situ generation of hydrogen peroxide, which is subsequently decomposed by the Cu SA sites to produce ·OH radicals that play a key role in the rate-determining step of methane activation to form methanol. Additionally, the presence of Cu SA not only enhances the electron-hole separation efficiency and improves the transfer of the photo-generated charges, but also increases the number of active sites for methane adsorption and activation. These insights provide valuable guidance for designing efficient catalysts for the highly selective photocatalytic oxidation of methane to methanol.
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SEPARATION AND PURIFICATION TECHNOLOGY
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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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Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Junfeng Zheng,Jinyu Liu,Zikang Qin,Yulei Ma,Yahui Yang,Linlin Yang,Hang He,Zhongde Dai,Wenju Jiang,Lin Yang,Lu Yao,Bo Tang
High water flux and dye rejection are crucial for effective textile wastewater treatment. In this study, novel two-dimensional (2D) metal-organic frameworks (MOFs) were synthesized and combined with one-dimensional (1D) halloysite nanotubes (HNTs) and polydopamine (PDA) to fabricate the thin-film nanocomposite (TFN) membranes. The surface morphology, chemical composition, and separation performance of resultant membranes were systematically characterized to illustrate their structure-property-performance relationships. Introducing hydrophilic 1D HNTs enhanced membrane hydrophilicity and bridged large gaps between the 2D MOF nanosheets. Under optimized conditions, the PDA-HNTs/MOFs membrane achieved a water permeance of 362.1 LMH·bar⁻¹ and 99.9 % rejection of Congo Red. PDA acted as a “bridge” linking HNTs and MOFs to the membrane substrate, thereby providing excellent antifouling performance and long-term stability. After 72 h of continuous operation, this membrane maintained a 99.1 % rejection of Congo Red, greatly surpassing both pure MOFs and HNTs/MOFs membranes. These findings highlight the superior filtration capabilities and promising potential of PDA-HNTs/MOFs membranes for dye wastewater treatment.
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Frontiers in Chemistry
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2025
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IF 4.2
Chen Yang,Yuanyuan Chen,Zhimin He,Rong Li,Xinglong Gou
The electrochemical nitrate reduction reaction (NITRR) offers a sustainable route for ammonia synthesis and environmental remediation but faces challenges such as sluggish kinetics and competing hydrogen evolution. This study aims to address these limitations by designing a Cu/molybdenum phosphide (MoP) heterostructure catalyst through one-pot calcination, which integrates Cu nanoparticles with MoP nanograins. Structural and electronic analyses confirm the formation of intimate Cu–MoP interfaces, where charge redistribution polarizes Cu to an electron-deficient state (Cuδ+) and enriches MoP with electrons. This configuration enhances nitrate adsorption on Cuδ+, while MoP efficiently supplies protons via accelerated water dissociation. The Cu/MoP catalyst achieves a record-high NH3 Faradaic efficiency (FE) of 98.93% and a yield rate of 30.72 mmol h−1 cm−2 at −0.5 V (vs. RHE), outperforming isolated Cu or MoP. When deployed in a Zn-nitrate battery, the composite cathode delivers a peak power density of 12.97 mW cm−2. This work provides a promising solution to the insufficient active hydrogen supply and poor NH3 conversion efficiency of Cu-based nitrate reduction catalysts.
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ACS Applied Nano Materials
·
2025
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IF 5.5
Yunjie Ren,Yueyuan Li,Min Qing,Yonghua Yuan,Jing Zhou,Lijuan Bai
Phosphate plays a crucial role in various physiological and pathological processes; however, effective strategies for analyzing diverse phosphates and monitoring phosphate hydrolysis remain limited. Herein, we develop a metal–organic framework wrapped Cu nanoclusters-based (CuNCs@MOF) fluorescent sensor array for high-throughput discrimination of phosphates and real-time monitoring of their enzymatic hydrolysis. Leveraging the confinement effect of zinc-based MOFs, the encapsulated CuNCs exhibited reduced intramolecular vibration and rotation, resulting in enhanced luminescence performance. Due to the distinct affinities of various phosphates toward zinc ions, the sensor array generates differentiated fluorescence responses for seven phosphates, including adenosine triphosphate (ATP), cytidine triphosphate, uridine triphosphate, adenosine diphosphate, adenosine monophosphate, pyrophosphate (PPi), and inorganic phosphate. Subsequently, the fluorescence response signals are processed using the pattern recognition algorithm to generate the unique fingerprint spectra of each phosphate. We demonstrate that the sensor array can not only identify seven distinct phosphates at concentrations as low as 5 μM and effectively distinguish between their mixtures but also exhibit excellent anti-interference capability and enable dynamic monitoring of ATP and PPi hydrolysis. Notably, the sensor array achieved outstanding performance in complex real-world samples and cellular-level analyses, demonstrating 100% accuracy in blind sample identification. Overall, this work develops a strategy for high-throughput discrimination of phosphates and real-time monitoring of their enzymatic hydrolysis.
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PROCESS SAFETY AND ENVIRONMENTAL PROTECTION
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2025
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IF 7.8
Yuan Chen,Dongdong Jia,Yu Gao,Wang Yuan,Yongyue Sun
To develop an efficient bifunctional material for bisphenol A (BPA) removal, a nitrogen-rich hierarchical porous Cu x @N-CM composite was synthesized by pyrolyzing Cu@ZIF-8 encapsulated with dicyandiamide (DCD). DCD introduced more pyridinic N, graphitic N, and Cu-N x active sites, and enhanced the material’s surface area and pore size. This unique structure endows the material with both superior adsorption capacity and peroxymonosulfate (PMS) activation ability, enabling efficient BPA removal from water. Specifically, after adsorption enrichment, 0.1 g L −1 of Cu x @N-CM can remove 75 % of BPA (20 mg L −1 ). Subsequent addition of 0.1 mmol L −1 PMS achieves complete BPA removal within 15 min. Furthermore, this material and process effectively minimize PMS consumption, exhibit a broad pH application range, and good cycling stability. Mechanistic studies show that adsorption occurs through pore filling, hydrophobic interactions, π-π electron donor-acceptor (EDA) interactions, and complexation. PMS activation is driven by radical and non-radical synergies. In addition, the adsorption active sites and PMS activation sites do not overlap, and the adsorption process prolongs the residence time of pollutants on the catalyst surface, thereby promoting the degradation process. This study provides valuable insights into designing catalysts for removing high-concentration, refractory organic pollutants from water.
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Applied Materials Today
·
2025
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IF 6.9
Zhenyu Li,Lingling Zhang,Yafei Chen,Xueyong Zheng,Chunli Jiang,Chunhua Luo,Hechun Lin,Hui Peng
The limitations of von Neumann architectures in computational speed and energy efficiency have driven the development of neuromorphic computing systems, where optoelectronic synaptic devices play a pivotal role in enabling brain-inspired information processing. This study presents an optoelectronic synaptic device based on a two-dimensional conductive metal-organic framework material Cu-BHT which exhibits broad visible-light absorption (300 - 600 nm), high photoconductivity, and solution processability. The fabricated device with a planar structure of Ag/Cu-BHT/Ag successfully simulates the key biological synaptic functionalities, including excitatory postsynaptic current (EPSC), paired-pulse facilitation (PPF), and short-to-long-term memory transitions. The device achieves a high accuracy of 96.3% in MNIST handwritten digit recognition using a convolutional neural network (CNN). Furthermore, multi-wavelength response of the device enables optical logic operations (AND/OR) and associative learning paradigms, such as Pavlovian conditioning experiment. This work underscores Cu-BHT as a versatile material for neuromorphic computing and artificial visual systems, with future research exploring scalable fabrication and hybrid integration to realize adaptive vision platforms with enhanced energy efficiency.
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