INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2024
·
IF 8.1
Jianing Mao,Guanghui Feng,Xiao Dong,Ziran Xu,Bingbao Mei,Yiheng Wei,Xiaohu Liu,Guihua Li,Shoujie Li,Yanfang Song,Fei Song,Wei Wei,Wei Chen,Zheng Jiang
CH 4 , as an important clean fuel and hydrogen carrier, its production from CO 2 driven by renewable energy could simultaneously achieve energy supply, CO 2 emission reduction, and renewable energy consumption, which is of great significance. Electrocatalytic CH 4 production relies on high-valence Cu species for realizing multielectron reduction, while facing inadequate performance stability due to the reconstruction tendency of Cu. Herein, an amorphous CuO x -SiO 2 catalyst (amorCuO x -SiO 2 ) is synthesized via an electrostatic interaction strategy to construct stable Cu 2+ active sites for efficient electrocatalytic CH 4 production. AmorCuO x -SiO 2 shows a good reconstruction resistance during electroreduction, confirmed via X-ray absorption spectroscopy studies, endowing a 63.7% CH 4 faradaic efficiency at 500 mA cm −2 , which is 7.8 folds of crystalized CuO x -SiO 2 (crysCuO x -SiO 2 ). Theoretical calculations revealed that stable Cu 2+ active sites enhanced *CO adsorption and were more susceptible for further hydrogenation, thus promoting the CO 2 -to-CH 4 conversion. Our findings provide a feasible strategy for developing reconstruction-resistant electrocatalysts for advanced CH 4 production performance.
研究领域:
材料科学
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环境科学
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DOI
高影响因子
Journal of Cleaner Production
·
2024
·
IF 9.7
Tao Chen,Chuan Ma,Ben Wang,Linlin Xu,Wu Yang,Lushi Sun
Pyrolysis has proven an effective method of recycling waste printed circuit boards (WPCBs) for high-value product generation. The kinetics and debromination studies on the pyrolysis of WPCBs with copper species was performed using a thermogravimetric-mass spectroscopy analyzer and a vertical quartz-tube reactor. A multiple distributed activation energy model (M-DAEM) was applied to illustrate the potential multiple reactions over the thermal decomposition process. The introduction of copper species into WPCBs reduced the initial activation energies, resulting in lower decomposition temperatures. Meanwhile, several distinct subprocesses were observed and resolved by three-reaction models. The addition of CuO obtained the lowest liquid yield (53.9 wt %) and the maximum gas yield (8.9 wt %), and the introduction of Cu 2 O resulted in the highest solid yield (40.4 wt %). Copper particles preserved 57 % of bromine in residual solid, while CuO and Cu 2 O particles resulted in approximately 65 % and 74 % retention of bromine in the residues, respectively. Particularly, less than 3.7 % of bromine was transferred into the liquid when Cu 2 O was added. The optimal debromination performance of Cu 2 O was attributed to its effective capture capacity of HBr/Br 2 , fairly high catalytic efficiency on dissociating C–Br bond, and multipath conversion of organobromine to cross-linked carbonaceous compounds.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Chengda Li,Yueli Wen,Bin Wang,Maohong Fan,Wenlong Liu,Zheng Cui,Wei Huang
Activation and desorption of the hydrogen atom in the toluene methyl is a restrictive step for side-chain alkylation of toluene with methanol (SATM). In this work, two dehydrogenation strategies were used to improve the catalytic performance, dehydrogenation component Cu was introduced in PAl-NaX catalyst as well as the acid-base property was adjusted by changing NaOH loading amount. The relationship among the percentage of acid-base sites, low valence Cu species and the catalytic performances was investigated combined with the multiple characterizations, like X-ray photoelectron spectroscopy (XPS), Temperature-programmed desorption (TPD) of NH 3 and CO 2 , etc. together with ternary regression analysis. It is found that the dehydrogenation component Cu, especially low valence Cu species, promotes the selectivity of side-chain alkylation products to a certain degree, but base sites play an even more critical role in enhancing it.
研究领域:
催化化学
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材料科学
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产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jingang Wang,Jianbo Zhang,Cheng Xing,Taosheng Jin,Jinpeng Liu,Meiting Ju,Xuejiao Tang
Phosphorus (P) poisoning of NH 3 -SCR catalysts is inevitable in application of NO x abatement of diesel exhaust. The distinct effects on Cu-SSZ-13 of P from different precursors (H 3 PO 4 and (NH 4 ) 2 HPO 4 ) were figured out and the mechanism was further investigated. P-poisoned Cu-SSZ-13 (Si/Al = 6) catalysts were prepared and characterized using N 2 adsorption, X-ray powder diffraction (XRD), scanning electron microscope with energy-dispersive X-ray spectroscopy mapping (SEM-EDX), ammonia temperature-programmed desorption (NH 3 -TPD), X-ray photoelectron spectroscopy (XPS), hydrogen temperature programmed reduction (H 2 -TPR), electron paramagnetic resonance (EPR) and 27 Al solid-state magic angle spinning nuclear magnetic resonance spectroscopies ( 27 Al NMR). Significant enhancement of high-temperature activities (400–600 °C) were observed for the catalysts with P loading of 0.3–0.9 wt%, since the appropriate incorporation enabled to bind P atoms to CuO x in remained framework. However, the high P content of 1.5 wt% resulted in a detrimental effect on framework to induce the accumulation of Cu species. Interestingly, the dominant P from H 3 PO 4 was inclined to directly attack the framework Al leading to more severe dealumination, while the P from (NH 4 ) 2 HPO 4 interacted with Cu 2+ to form copper phosphate with more Cu 2+ migrating to the surface of the catalyst which promoted the NO x conversation at each active site resulting in the low-temperature catalytic activity unchanged. So, control of the P/Cu and form of P is capable of preventing P poisoning and unlocks the potential of Cu-SSZ-13 in exhaust treatment.
研究领域:
环境科学
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催化化学
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产品关联
DOI
高影响因子
ACS Catalysis
·
2024
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IF 11.3
Mei-Yao Wu,Shan-Qing Li,Wei-Wei Wang,Chun-Jiang Jia
The structures of active components in practical solid catalysts are seldom homogeneous, which makes it challenging to explore the synergistic effect among the complex catalyst components in heterogeneous catalysis. The active structure of Cu-based catalysts, which are widely used in water gas shift reactions and other important industrial reactions, has been debated. This work prepared Cu–MgO catalysts with the copresence of Cu particles and Cu atoms to investigate the synergistic effects of these Cu species. We found that the Cu nanoparticles served to adsorb and activate the reactant molecule of CO, while the atomic Cu species at the surface of the MgO lattice might exist as the Mg2Cu2–Ov site for water dissociation. The presence of surface-substituted Cu atoms modulated the reactivity of adjacent oxygen vacancy in the MgO surface, enhanced the ability of H2O dissociation to form reactive –OH species, and allowed the oxygen vacancies to recycle, contributing to the continuation of the reaction. A volcano-type relation of catalytic performance versus Cu0/Cu2+ ratio has been established, revealing the existence of synergy between Cu particles and Cu atoms. In addition, due to this synergistic effect, the optimized Cu–MgO catalyst shows a very high activity with a CO conversion rate of 1119 μmolCO gCu–1 s–1 at 300 °C. This work revealed the synergistic effect of different Cu species in the Cu–MgO catalysts, which was important for unraveling the contribution of complex components to catalytic performance.
研究领域:
催化化学
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材料科学
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DOI
高影响因子
RSC Advances
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2017
·Vol. 7
·期 60
·37787-37796
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IF 3.108
Xuesong Liu,Xiaodong Wu,Duan Weng,Zhichun Si,Rui Ran
Cu/SAPO-34 catalysts were prepared by wet impregnation and ion-exchange methods, and both the catalysts were hydrothermally treated at 750 °C in 10 vol% H2O/air for 24 h. Subsequently, the as-received and hydrothermally treated catalysts were exposed to a sulfur poisoning treatment at 350 °C in 100 ppm SO2/10 vol% H2O/air for 24 h and examined for NOx conversion. Sulfur poisoning considerably decreased the NOx conversion efficiency of the catalysts at low temperatures. In contrast, it improved the high-temperature selective catalytic reduction (SCR) activities of the as-received catalysts. The ion-exchange-prepared catalysts displayed higher sulfur tolerance than the impregnation-prepared catalysts at 150–350 °C. The electron paramagnetic resonance, X-ray photoelectron spectroscopy, energy-dispersive X-ray spectroscopy and H2-temperature-programmed reduction results showed that sulfur poisoning significantly influenced the migration of the copper species and thereby the amount of active isolated Cu2+. More dispersed CuSO4 was produced on the ion-exchange-prepared catalysts than on the impregnation-prepared catalysts after sulfur poisoning. The dispersed CuSO4 showed considerably higher SCR activity than the crystalline CuSO4. Both the dispersed CuSO4 and remaining isolated Cu2+ determined the low-temperature SCR behavior of the sulfur-poisoned catalysts.
研究领域:
催化化学
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环境科学
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DOI
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
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2022
·Vol. 30
·期 6
·15991-16002
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IF 5.19
Zhang Xueying,Liu Yonggang,Yu Yonghao,Wang Lifen,Lin Yinjun
Here, we report a simple and efficient strategy for evenly in situ growth of Cu 2 (OH) 3 F nanosheets on BiVO 4 spheres as a novel photo-Fenton-like catalyst using hydrothermal method. The Cu 2 (OH) 3 F/BiVO 4 composite catalysts showed great performance for the organic pollutants degradation under visible light irradiation due to the efficient electron transfer and copper species transformation. The synergetic between Cu 2 (OH) 3 F and BiVO 4 not only promoted the separation of electrons and holes but also enhanced the Cu 2+ reduction, thus produced more strong oxidative radicals under a wide pH value range. The activity of Cu 2 (OH) 3 F/BiVO 4 composite for methylene blue degradation was 6.03 and 5.47 times more than that of pristine Cu 2 (OH) 3 F and BiVO 4 , respectively. The composite catalysts were characterized with various methods and their stability and adaptability were also evaluated. Finally, a possible photo-Fenton-like reaction mechanism was also proposed based on the band structure/position and reaction species.
研究领域:
环境科学
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材料科学
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF RARE EARTHS
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2017
·
IF 2.429
Linying Du,Weiwei Wang,Han Yan,Xu Wang,Zhao Jin,Qisheng Song,Rui Si,Chunjiang Jia
Copper-ceria sheets catalysts with different loadings of copper (2 wt.%, 5 wt.% and 10 wt.%) supported on ceria nanosheets were synthesized via a deposition–precipitation (DP) method. The prepared catalysts were systematically characterized with various structural and textural detections including X-ray diffraction (XRD), Raman spectra , transmission electron microscopy (TEM), X-ray absorption fine structure (XAFS), and temperature-programmed reduction by hydrogen (H 2 -TPR), and tested for the CO oxidation reaction. Notably, the sample containing 5 wt.% of Cu exhibited the best catalytic performance as a result of the highest number of active CuO species on the catalyst surface. Further increase of copper content strongly affects the dispersion of copper and thus leads to the formation of less active bulk CuO phase, which was verified by XRD and H 2 -TPR analysis. Moreover, on the basis of in-situ diffuse reflectance infrared Fourier transform spectroscopy ( in-situ DRIFTS) results, the surface Cu + species, which are derived from the reduction of Cu 2+ , are likely to play a crucial role in the catalyzing CO oxidation. Consequently, the superior catalytic performance of the copper-ceria sheets is mainly attributed to the highly dispersed CuO x cluster rather than Cu-[O x ]-Ce structure, while the bulk CuO phase is adverse to the catalytic activity of CO oxidation.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
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2025
·
IF 3.3
Xue-Qing Xu,Shen Yu,Xing-Yu Yue,Zhan Liu,Jia-Min Lyu,Yi-Long Wang,Zhi-Yi Hu,Yu Li,Li-Hua Chen,Bao-Lian Su
Phenol is an important intermediate for high value chemicals. Current phenol production via a three-step cumene process causes severe energy-waste and environmental problems. The conversion of benzene to phenol under mild condition can be achieved by oxidation with Cu-based zeolites. However, conventional microporous zeolite suffers from severe diffusion limitation, especially when bulky molecules are involved, such as benzene. In this work, we used a hierarchically macro-meso-microporous ZSM-5 single crystal (Hier-ZSM-5) as substrate for Cu species (Cu@Hier-ZSM-5). Irregular morphology of opal-like Hier-ZSM-5 exhibits abundant surface Si-OH groups and provides a platform for stabilizing Cu2+ sites. Meanwhile, hierarchical porosity provides significantly improved diffusion ability of bulky molecules. As a result, excellent selective oxidation performance of benzene was obtained with the Cu@Hier-ZSM-5, achieving a conversion of 77% and a phenol selectivity of 73%, which is 1.5 times and 2 times of these obtained with a catalyst based on a microporous ZSM-5, respectively. Species of CuOOH were identified as an important intermediate for benzene oxidation. This hierarchical zeolite system with a synergistic effect of site anchoring and molecular diffusion presents an excellent platform for catalyst design.
研究领域:
催化化学
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材料科学
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环境化学
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产品关联
DOI
PubMed
高影响因子
Acta Geochimica
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2025
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IF 1.3
Wang Zhenglong,Shang Linbo,Chou I-Ming,Chen Chen,Zhou Yunhe,Li Jianguo,Jiang Ziqi,Gao Xinwei,Wan Ye
The formation of copper deposits is closely related to hydrothermal processes. Understanding the migration of copper in hydrothermal fluids aids in reconstructing mineralization processes and deciphering deposit genesis. Copper primarily exists as Cu + and Cu 2+ in hydrothermal solutions, with redox conditions governing their interconversion. In chloride-rich geological fluids, Cu–Cl complexes are considered critical for copper transport. However, the specific types and valence transitions of Cu–Cl complexes under varying hydrothermal conditions remain poorly understood. This study employed in situ Raman spectroscopy to systematically analyze Cu + HCl and CuCl 2 + K 2 S 2 O 3 /H 2 systems under saturated vapor pressure at 25–300 °C, elucidating the effects of temperature, Cl − concentration, and redox conditions on copper speciation. In the Cu + HCl system, copper dissolved as monovalent Cu–Cl complexes. At high temperatures (> 200 °C), [CuCl 2 ] − is the dominated species, whereas [CuCl 3 ] 2− becomes prevalent at lower temperatures and higher HCl concentrations. For the Cu 2+ –Cl system, the dominant species transitioned from [Cu(H 2 O) n ] 2+ (< 50 °C) to [CuCl 4 ] 2− (100 °C) and further to [CuCl] + and [CuCl 2 ] 0 at 300 °C. The introduction of reducing agents (K 2 S 2 O 3 /H 2 ) facilitated Cu 2+ → Cu + reduction, thereby stabilizing Cu + –Cl complexes and inducing partial copper precipitation. The behavior of copper in chloride-rich hydrothermal fluids observed in this study indicates that high-temperature oxidizing fluids facilitate Cu mobilization, while cooling and redox changes promote deposition and ore minerals formation.
研究领域:
矿物学
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地球化学
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产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2020
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IF 8.758
Ting Chen,Zhiliang Zhu,Hua Zhang,Yanling Qiu,Daqiang Yin,Guohua Zhao
Heterogeneous catalysis can be enhanced through the construction of effective atom connection for rapid electron transport on the catalyst surface. Hence, this study proposed a new strategy for electron transfer regulation to facilitate redox cycle of Cu(II)/Cu(I). The objective was achieved by successful construction of copper-containing covalent bond through the in situ growth of porous g-C3N4 with oxygen dopants and nitrogen defects (O-CND) on CuAlxOy substrate (CuAl@O-CND). On the basis of X-ray absorption fine structure (XAFS) and other characterization results, the facilitated redox behavior of copper species by electron transfer regulation was ascribed to the formation of a C–O–Cu bond on the porous-rich superficial of the catalyst; these covalent C–O–Cu bonds shortened the migration distance of electrons between Cu(II) and Cu(I) via Cu(I)–O–C–O–Cu(II) bridge. The construction of copper-containing covalent bonds in the catalyst resulted in efficient PMS activation for a rapid redox cycle of Cu(II)/Cu(I), triggering a series of reactions involving the continuous production of three highly active species (SO4·–, ·OH and 1O2). The rapid diffusion and transportation of the generated active species from porous structures directly attack typical pharmaceutically active compounds (PhACs), achieving superior catalytic performance. This study provides a new routine to construct a C–O–Cu bond for PMS activation by regulating the electron transfer to accelerate the redox behavior of copper species for environmental remediation.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Yue Ma,Songqi Cheng,Xiaodong Wu,Tongxi Ma,Liping Liu,Baofang Jin,Minghan Liu,Jianbo Liu,Rui Ran,Zhichun Si,Duan Weng
To improve the hydrothermal durability of Cu-SSZ-13 selective catalytic reduction (SCR) catalyst, a thin Al 2 O 3 modification layer was coated on the external surface of Cu-SSZ-13 by a chemical liquid deposition (CLD) method. The high-temperature SCR activity of the Al-modified Cu-SSZ-13 can be maintained upon 750–800 °C hydrothermal aging, and over-oxidation of NH 3 is largely inhibited. Based on H 2 -TPR and EPR results, it is revealed that CuAl 2 O 4 -like species forms upon Al modification and converts further to CuAlO 2 -like species during aging, while the accumulation of CuO-like species is inhibited. The high affinity of Al-containing species ( i.e. , Al 2 O 3 and CuAl 2 O 4 -like species) with Cu(OH) 2 is suggested by DFT calculations, indicating that Cu(OH) 2 detached from ion-exchange sites are captured by Al to form CuAlO 2 -like species instead of CuO-like species. The passivation of detached Cu species by coated Al leads to somewhat weakened low-temperature SCR activity, but successfully preserves the high-temperature SCR performance upon aging, which can be applied to high-temperature SCR scenarios.
研究领域:
催化化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）