JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
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IF 9.4
Feng Yue,Mengke Shi,Cong Li,Yang Meng,Shuo Zhang,Lan Wang,Yali Song,Jun Li,Hongzhong Zhang
Directly capturing CO 2 in ambient air and converting it into value-added fuels using photocatalysis is a potentially valuable technology. In this study, Cu-porphyrin (tetrakis-carboxyphenyl porphyrin copper, CuTCPP) was innovatively anchored on the surface of TiO 2 (titanium dioxide) nanosheets to form an S-scheme heterojunction. Based on this, a photocatalytic reaction system for stably converting CO 2 in ambient air into value-added fuels at the gas–solid interface was constructed without addition of sacrificial agents and alkaline liquids. Under the illumination of visible light and sunlight, the evolution rate of CO is 56 μmol·g −1 ·h −1 and 73 μmol·g −1 ·h −1 , respectively, with a potential CO 2 conversion rate of 35.8 % and 50.4 %. The enhanced of photocatalytic performance is attributed to the introduction of CuTCPP, which provides additional active sites, significantly improves capture capacity of CO 2 and the utilization of electrons. Additionally, the formation of S-scheme heterojunction expands the redox range and improves the separation efficiency of photo-generated charges.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Lixian Wang,Lizhi Zhao,Xianglong Xiao,Xiaofu Wang,Jiayi Cao,Hui Ye,Hong Li,Yuzhong Zhang
Wastewater discharged from the textile industry contains large amounts of dyes and salts, causing serious pollution to the environment. Loose nanofiltration (LNF) membranes offer a promising solution for dye/salt separation. However, membrane fouling is a critical issue affecting the membrane performance. Here, polyether amine (PEA) is used as the aqueous monomer for interfacial polymerization to prepare a polyamide (PA) LNF membrane, and peroxidase-like Cu-FeTCPP nanosheets are embedded into the PA layer to develop the Nanozyme@PA membrane. The nanozyme-incorporated membrane has a thinner and enhanced porous active layer than PA membrane, resulting in higher water permeance (maximum of 80.7 L·m −2 ·h −2 ·bar −1 ), notable rejection of dyes (CR, >99.2 %) but low rejection of inorganic ions (NaCl, <6.4 %). The optimum dye/salt separation factor of Nanozyme@PA reaches 218.7. The loaded nanozyme can catalyze the degradation of dyes adsorbed on the membrane surface in the presence of hydrogen peroxide within 10 min, without the need for special operation, enabling the recovery of water permeance. This nanozyme functionalized LNF membrane with good permeability, selectivity and self-cleaning offers an efficient approach to dye wastewater treatment as well as an insight for membrane fabrication assisted by two-dimensional nanozyme.
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APPLIED SURFACE SCIENCE
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2024
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IF 6.3
Longlong Geng,Fengting Geng,Xianghan Cheng,Xiaoli Wang,Ling Wang,Xuliang Pang,Yong-Zheng Zhang,Xiuling Zhang,Da-Shuai Zhang,Shujuan Zhuang,Abdukader Abdukayum,Guangzhi Hu
Copper is a crucial element in the field of catalysis. However, Cu-based catalysts exhibit lower redox properties and surface energy under mild conditions, which limit their electron transfer capacities and catalytic performance. In this study, the relationship investigation between the hydrogenation behavior of Cu-based catalysts and crystal phases showed that spherical Cu 2 O exhibited enhanced capacity for hydrogen activation, excellent catalytic activity and outstanding reusability in the selective reduction of various nitroarenes. At even 25 °C and 1 atm, the complete reduction of 4-nitrophenol by NaBH 4 was achieved in 2.5 min over Cu 2 O, achieving a reaction rate constant ( k ) of 20.15 × 10 −3 s −1 , which was 4.8 and 15.2 times that of CuO and Cu catalysts. Detailed experimental and theoretical calculations revealed that the Cu + sites in the antifluorite crystal phase of Cu 2 O are conducive to the adsorption of active H species, while the unique d–s orbital recombination provides more electrons to improve its hydrogenation performance. The results of this study can aid in the development of copper-based materials as advanced catalysts, thereby improving fine chemical production and pollution treatment processes.
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Journal of the American Chemical Society
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2024
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IF 14.4
Chang Long,Kaiwei Wan,Yu Chen,Lei Li,Yuheng Jiang,Caoyu Yang,Qianbao Wu,Guoling Wu,Peng Xu,Jiong Li,Xinghua Shi,Zhiyong Tang,Chunhua Cui
As fuel and an important chemical feedstock, n-propanol is highly desired in electrochemical CO2/CO reduction on Cu catalysts. However, the precise regulation of the Cu localized structure is still challenging and poorly understood, thus hindering the selective n-propanol electrosynthesis. Herein, by decorating Au nanoparticles (NPs) on CuO nanosheets (NSs), we present a counterintuitive transformation of CuO into undercoordinated Cu sites locally around Au NPs during CO reduction. In situ spectroscopic techniques reveal the Au-steered formation of abundant undercoordinated Cu sites during the removal of oxygen on CuO. First-principles accuracy molecular dynamic simulation demonstrates that the localized Cu atoms around Au tend to rearrange into disordered layer rather than a Cu (111) close-packed plane observed on bare CuO NSs. These Au-steered undercoordinated Cu sites facilitate CO binding, enabling selective electroreduction of CO into n-propanol with a high Faradaic efficiency of 48% in a flow cell. This work provides new insight into the regulation of the oxide-derived catalysts reconstruction with a secondary metal component.
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Molecular Catalysis
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2024
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IF 3.9
Zheng Zhou,Meng Miao,Wenzhi Li,Jingting Jin,Liqun Wang,Lulu Zhang,Liang Yuan
The selective conversion of methane is a significant but difficult challenge. We reported a CuFe bimetallic catalyst supported by g-C 3 N 4 for the catalytic oxidation of methane to oxygenated C1 products. Using H 2 O 2 as the oxidant, Cu 0.4 Fe 0.3 -C 3 N 4 catalyst had a C1 yield of 8231 μmol·g cat −1 · h −1 at 70 °C, and 1 H NMR results showed that almost all of the liquid phase products were target C1 products. The methanol selectivity on CuFe-C 3 N 4 was 44.5 %, comparing with 20.2 % methanol selectivity on Cu-C 3 N 4 . The formation of a Cu-O-Fe site on the CuFe-C 3 N 4 was confirmed by in situ DRIFTS and 57 Fe Mössbauer spectroscopy. This Cu-O-Fe site was responsible for the improved catalyst performance. DFT calculations illustrated that at the Cu-O-Fe site, H 2 O 2 dissociated into two ·OH radicals instead of ·H and ·OOH radicals as it did at the Cu-O-Cu site. The ·OH radicals combined with the ·CH 3 radicals from the CH 4 molecules to form methanol. These findings provided valuable insights into the rational design of active sites on carbon nitride materials.
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Small
·
2024
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IF 13
Yi Shen,Yongliang Pan,Chao Zhu,Haizhong Zhang,Jun Wang,Renlan Liu,Qile Fang,Shuang Song,Baoliang Chen
In the domain of heterogeneous catalytic activation of peroxymonosulfate (PMS), high-valent metal-oxo (HVMO) species are widely recognized as potent oxidants for the abatement of organic pollutants. However, the generation selectivity and efficiency of HVMO are often constrained by stringent requirements for catalyst adsorption sites and electron transfer efficiency. In this study, a single-atom catalyst, Cu SA /CN P&S, is synthesized featuring multiple types (planar/axial) of heteroatom coordination via an H-bond-assisted self-assembly strategy. It is confirmed that CuN 3 active centers with axial S coordination are uniformly distributed in a carbon matrix modified by planar P atoms. Cu SA /CN P&S activated PMS to selectively generate Cu (III) ═OH species as the primary reactive oxygen species (ROS). The pseudo-first-order kinetic rate for bisphenol A degradation reached 1.51 min −1 , a 17.57-fold increase compared to the unmodified Cu SA /CN catalyst. Additionally, the Cu SA /CN P&S catalyst demonstrates high efficiency and durability in removing contaminants from various aqueous matrices. Theoretical calculations and experimental results indicate that the intrinsic electric field generated by distal planar P atoms enhances electron transfer efficiency within the carbon matrix. Meanwhile, axial S coordination elevates the d-band center and tunes the e g * band broadening of Cu, thereby enhancing the adsorption selectivity for the terminal oxygen of PMS. This multitype coordination synergistically mitigates the issues of low selectivity and yield of HVMO species.
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SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Jihan Lu,Xuanting He,Boyu Li,Shuang Meng,Zhuo Li
Developing multifunctional and super-wetting separation materials is of great significance for treating complex oily wastewater in real environment. Herein, the superhydrophilic Cu-HHTP@Cu foam with hierarchical structure was fabricated by chemical oxidation and in situ growth strategies, which showed an outstanding separation efficiency (>99.4 %) and flux (>92.1 kL∙m −2 ∙h −1 ) for various oil/water mixtures. The electrostatic attraction, π − π interactions and hydrogen bonding between Cu-HHTP@Cu foam and dyes facilitate the adsorption process, with a removal efficiency > 94.7 %. To absorb high-viscosity crude oil, the Cu-HHTP@Cu foam was further modified with polydimethylsiloxane (PDMS) to finally obtain superhydrophobic PDMS@Cu-HHTP@Cu foam, which demonstrates high separation efficiency (>99.8 %) and flux (>90.3 kL∙m −2 ∙h −1 ). Both Cu-HHTP@Cu foam and PDMS@Cu-HHTP@Cu foam also showed stable durability after 20-cycle tests. More importantly, due to the introduction of Cu-HHTP, PDMS@Cu-HHTP@Cu foam presented excellent photothermal conversion behavior with the surface temperature reaching up to 72.0℃ under simulated sunlight, which remarkably facilitate the cleaning of crude oil. This work shows that modified Cu foam is a promising candidate for absorbing dyes and treating crude oil spills and is expected to provide a convenient method for oil/water separation.
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Journal of Materials Chemistry A
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2025
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IF 9.5
Yue Chen,Yu Ma,Chen Liao,Jiacheng You,Huihuang Fang,Chongqi Chen,Yu Luo,Lilong Jiang
The construction and stabilization of Cu–O–Si interfaces in copper-based catalysts remain critical yet challenging for the water-gas shift reaction (WGSR), as conventional strategies fail to mitigate copper nanoparticle (NP) aggregation and interfacial instability. This study innovatively proposes a spatial confinement strategy by anchoring Cu NPs inside (Cuin/SBA-15) or outside (Cuout/SBA-15) the mesoporous channels of SBA-15, leveraging nanoscale confinement to optimize Cu–O–Si interfaces. The confined Cuin/SBA-15 catalyst demonstrated exceptional WGSR performance, achieving a reaction rate of 5.4 μmolCO·gcat−1·s−1, significantly surpassing conventional Cu/SBA-15 (3.1 μmolCO·gcat−1·s−1) and surface-loaded Cuout/SBA-15 (2.8 μmolCO·gcat−1·s−1), along with remarkable stability. This enhancement originates from the SBA-15 channels enabling the in situ formation of stable Cu–O–Si interfaces, which regulate the dynamic equilibrium between Cu0 (active for H2O dissociation) and Cu+ (critical for CO adsorption) species. In situ studies revealed their synergistic dynamic interconversion during WGSR, while domain confinement effects suppressed sintering by maintaining interfacial integrity. Kinetic and mechanistic analyses further identified the associative pathway, with HCOO* intermediate dissociation as the rate-determining step, facilitated by the stabilized Cu–O–Si interfaces. By resolving interfacial instability through confinement engineering, this work provides a paradigm for designing robust Cu-based catalysts, advancing both fundamental understanding and practical applications in WGSR and related heterogeneous catalysis.
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JOURNAL OF HAZARDOUS MATERIALS
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2025
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IF 11.3
Yao Ji,Tiangang Ma,Xianwang Yang,Renshuo Wang,Ke Wang,Xiyu Liu,Xiaolong Wang,Quan Jin
SO 2 sensors generally face challenges such as gas corrosion, poor selectivity, competition from water molecules, and high recovery costs. Metal-organic frameworks (MOFs), which offer excellent chemical stability, structural diversity, and low-cost reactivation, have emerged as ideal candidates for sensing materials. However, MOFs typically exhibit poor conductivity, making them unsuitable for traditional gas detection devices. In order to solve this problem, in this study, SIFSIX-1-Cu with directionally ordered interconnected nanochannels was synthesized. By optimizing the synergistic effects of mass transfer, chemical recognition and pore-size sieving, the performance limitations of traditional adsorption materials have been overcome. Furthermore, by integrating SIFSIX-1-Cu with a microwave circuit, the microwave gas sensor (MGS) detects target gases by monitoring changes in the electromagnetic properties—such as dielectric constant or resonance frequency—of the sensing material induced by gas adsorption. The unique detection mechanism allows the MOFs to operate without the need for conductivity optimization, effectively preventing the loss of active sites during the material modification process. The results showed that SIFSIX-1-Cu microwave gas sensor has a low limit of detection of 8.9 ppb at room temperature, and can achieve high selectivity (selectivity coefficient SO 2 /CO 2 > 11.87) detection of SO 2 in a wide concentration detection range of 10 ppb to 1000 ppm. Meanwhile, the sensor also exhibits excellent moisture resistance and repeatability.
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Environmental Technology & Innovation
·
2025
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IF 7.1
Shuzhen Yang,Bingjing Tian,Yanfang Huang,Bingbing Liu,Shengpeng Su,Wenjuan Wang,Guihong Han
The persistent dye rhodamine B (RhB) in textile wastewater poses severe ecological threats, demanding efficient and sustainable treatment technologies. This study synthesized a novel trimetallic Cu-Fe-Co catalyst via a nitrogen-atmosphere co-reduction method. The catalyst’s unique advantage lies in the synergistic effects of Cu, Fe, and Co, which significantly enhance catalytic performance. The redox-active phases of Cu, combined with the Fenton-like reactivity of Fe, are further optimized by Co doping to improve reactive oxygen species (ROS) generation and electron transfer efficiency. Characterization revealed a dendritic structure dominated by Cu, Cu₂O, and FeO phases, with Co-induced lattice expansion (Δ d / d = +0.25 %) enhancing surface reactivity. Under optimized conditions (pH 3, 1.5 g/L catalyst, 20 mg/L RhB), the ternary Cu-Fe-Co catalyst achieved 99.8 % RhB degradation within 40 min, with high mineralization efficiency (46.5 % TOC removal, 82.1 % COD removal). Mechanistic studies demonstrated that Co incorporation promotes the conversion of superoxide radicals (·O₂⁻) into long-lived singlet oxygen (¹O₂), synergistically enhancing oxidative effects from ·OH and ¹O₂, while in situ H₂O₂ generation drives radical chain reactions. Compared to binary catalysts, the ternary system exhibits superior degradation kinetics for RhB and maintains 95.8 % degradation efficiency even after five cycles. This study provides new insights into trimetallic catalyst design, highlighting its practical potential for wastewater treatment.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Guozhu Gao,Yong Zhang,Feifei Chen,Meiqin Xu,Chang Sun,Yangfan Song,Weihua Wang,Feng Lu,Hong Dong,Hui Liu,Yahui Cheng
Copper-based catalysts have been established as highly effective for facilitating the electrochemical reduction of carbon dioxide (ECO 2 RR), particularly in the synthesis of multi-carbon (C 2+ ) compounds. However, issues of product selectivity and reaction stability persist, posing significant challenges in the context of high-current-density industrial applications. In this study, we introduce a Cu-enriched Cu 3 N composite catalyst, synthesized via a straightforward magnetron sputtering technique. This catalyst is capable of activating CO 2 and efficiently adsorbing CO, thereby enhancing the electrocatalytic performance for the targeted reactions. At a potential of −1.2 V vs. RHE, the Faradaic efficiency (FE) of the C 2+ product reaches the highest value of 80.39 % with the current density of 267.78 mA cm −2 . Remarkably, the precisely engineered catalyst architecture integrated with a metallic copper (Cu) protective layer demonstrates significantly enhanced ECO 2 RR stability, maintaining C 2+ FE above 79 % for over 10 h at 200 mA cm −2 current density. These results provide a feasible approach for designing and implementing efficient and stable ECO 2 RR catalysts to generate C 2+ products for industrial applications.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
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IF 9
Fanjing Wei,Weizhou Jiao,Bo Liu,Hao Qin,Guisheng Qi,Jing Guo,Zhiguo Yuan,Liping Chang,Junjie Liao,Ting Li
Cu-ZnO is a promising sorbent for the removal of thiophene. However, the aggregation and growth of copper grains during the heating reaction leads to the sintering deactivation of the sorbent. Although various strategies have been proposed to introduce supports to mitigate these defects, the impact of supports on the desulfurization performance of sorbent remains poorly understood. In this study, Cu-ZnO/Al 2 O 3 sorbents were synthesized with excellent performance by incorporating Al 2 O 3 (derived from Al(NO 3 ) 3 , γ-Al 2 O 3 and AlOOH as aluminum sources) using co-precipitation and fractional precipitation methods. The thiophene removal evaluation was conducted in a fixed bed reactor. The results indicates that the breakthrough adsorption capacity for thiophene ( Q b-thiophene ) of sorbent synthesized using γ-Al 2 O 3 and AlOOH is approximately 25 % higher than that of those synthesized with Al(NO 3 ) 3 . In comparison to Al(NO 3 ) 3 , γ-Al 2 O 3 and AlOOH exert less influence on the precipitation and crystallization processes of Cu 2+ and Zn 2+ . Sorbents synthesized with γ-Al 2 O 3 and AlOOH as aluminum sources demonstrate higher copper dispersion, larger specific surface area and smaller grain size, all of which significantly enhance the desulfurization activity of sorbent. Furthermore, the use of γ-Al 2 O 3 and AlOOH as aluminum sources contributes to an increase in ZnO and unsaturated Zn δ+ contents on sorbent surface. This improvement enhances hydrogen storage capacity and promotes hydrogen spillover at the Cu-ZnO interface; additionally, it facilitates both the adsorption activation of thiophene and the stable fixation of sulfur species. These findings provide an important theoretical basis for the design and large-scale application of efficient desulfurization sorbents.
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