ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Kaicheng Qian,Tong Wei,Xiaoqing Yan,Dongming Qi,Mingwu Tan,Renhong Li
Element doping is a viable strategy to regulate the metal–support interface for enhancing the catalytic performance of supported metal catalysts. Herein, Cu/ZnO:Cu-TH catalysts are prepared by immobilizing Cu nanoparticles (NPs) on ZnO nanorods featuring an adjustable oxygen vacancy, in which partial Cu atoms at the Cu–ZnO interface are incorporated into the ZnO lattice to form CuxZn1–xO species. Such Cu atom doping induces the creation of distinctive Cu–CuxZn1–xO interface sites and optimizes electron transfer from ZnO to Cu NPs, thereby achieving intermediate activation and ultimately endowing the catalyst with superior performance in reforming alkali-free formaldehyde (HCHO) into hydrogen at low temperatures. The Cu–CuxZn1–xO interface sites serve as pivotal centers for HCHO reforming, where the Cu sites and CuxZn1–xO sites selectively engage in the cleavage of C–H bonds in HCHO and O–H bonds in H2O, respectively. Meanwhile, the presence of oxygen vacancies bolsters the Cu–CuxZn1–xO sites in enhancing the adsorption of HCHO and H2O, further improving the activity. The Cu/ZnO:Cu-450H catalyst, distinguished by abundant Cu–CuxZn1–xO sites and a high concentration of oxygen vacancies, demonstrates optimal activity with TOF values of 16.9 and 72.4 h–1 under anaerobic and aerobic conditions, respectively, which are 8.9 and 29.0 times higher than those of the Cu/ZnO-450N catalyst, which lacks doped Cu atoms and oxygen vacancies.
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Advanced Science
·
2024
·
IF 14.3
Jin Li,Qiuling Jiang,Xiujing Xing,Cuilian Sun,Ying Wang,Zhijian Wu,Wei Xiong,Hao Li
Electrochemical conversion of nitrate (NO 3 − ) to ammonia (NH 3 ) is a potential way to produce green NH 3 and remediate the nitrogen cycle. In this paper, an efficient catalyst of spherical CuO made by stacking small particles with oxygen-rich vacancies is reported. The NH 3 yield and Faraday efficiency are 15.53 mg h −1 mg cat −1 and 90.69%, respectively, in a neutral electrolyte at a voltage of -0.80 V (vs. reversible hydrogen electrode). The high activity of the electrodes results from changes in the phase and structure during electrochemical reduction. Structurally, there is a shift from a spherical structure with dense accumulation of small particles to a layered network structure with uniform distribution of small particles stacked on top of each other, thus exposing more active sites. Furthermore, in terms of phase, the electrode transitions from CuO to Cu/Cu(OH) 2 . Density functional theory calculations showed that Cu(OH) 2 formation enhances NO 3 - adsorption. Meanwhile, the Cu(OH) 2 can inhibit the competing hydrogen evolution reaction, while the formation of Cu (111) crystal surfaces facilitates the hydrogenation reaction. The synergistic effect between the two promotes the NO 3 - to NH 3 . Therefore, this study provides a new idea and direction for Cu-based oxides in electrocatalytic NH 3 production.
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JOURNAL OF NANOSCIENCE AND NANOTECHNOLOGY
·
2020
·Vol. 20
·期 3
·1660-1669
·
IF 1.134
Deng Yu-Ying,Xiao Xin-Feng,Wang Dan,Han Bo,Gao Yu,Xue Jian-Liang
Cu-BTC was synthesised by hydrothermal method in this study to adsorb and remove the toxic heavy metal hexavalent chromium Cr(VI) in water. The EDTA-chitosan/Cu-BTC was prepared by the surface modification of Cu-BTC with EDTA-modified chitosan. The initial concentration effects of adsorbed
chromium solution, adsorbent dosage, adsorption time, adsorption temperature and pH of chromium solution on adsorption capacity were estimated using the single-factor optimisation experiment. Results show that the adsorption capacity of the modified composite was higher than that of Cu-BTC.
Cu-BTC and EDTA-chitosan/Cu-BTC exhibited significant adsorption of Cr(VI) under acidic conditions in water and basically independent of temperature. Their adsorption processes conformed with the pseudo-second-order model. The Langmuir adsorption isotherm model obtained the adsorption isotherm,
which indicated that the adsorption process was single molecule adsorption. Isotherm fitting obtained the maximum adsorption amounts of Cr(VI) for Cu-BTC and EDTA-chitosan/Cu-BTC at 27.32 and 46.51 mg·g-1, respectively. Factor and principal component analyses show that the
main factors affecting the adsorption of Cr(VI) in the EDTA-chitosan/Cu-BTC composites are pH, initial concentration and adsorption time. Therefore, EDTA-chitosan-modified Cu-BTC was a more feasible metal-organic framework material than Cu-BTC because of better adsorption performance, which
can be used for adsorption removal of Cr(VI) in water.
研究领域:
环境科学
·
材料科学
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SENSORS AND ACTUATORS B-CHEMICAL
·
2021
·
IF 7.46
Jialing Zhou,Hui Huang,Shunji Chen,Mengyuan Wang,Danna Zhao,Jun Yu,Senlin Jin,Yuan Zhong,Xiaoming Chen,Xiaocai Yu,Pengbo Liu,Jian Zhao
As 3rd generation semiconductor, GaN material is promising for biosensor application, owing to its excellent chemical stability and high carrier mobility. Herein, GaN porous-layer (GNP) was self-assembly grown on GaN-coated sapphire substrate without doping by using simple low-temperature (LT) growth. The GNP with a pore density as high as ∼2.1 × 10 3 μm −2 can be realized by optimizing the growth temperature (620 °C) and layer thickness (22.4 nm), and its normalized conductivity can be tuned by simply changing the thickness. The optimized GNP was applied to chemiresistive detection of Cu 2+ with a limit of detection (LOD) as low as 8 fM, a fast response speed of 1.5 min, a wide linear range (8 fM∼8 nM) and good repeatability. The LOD was improved 1.25∼10 6 fold compared with that of previously reported biosensor. The GNP biosensor features high sensitivity, simple structure, integratability, and low-cost. To our knowledge, it is the first time that GaN material was used for chemiresistive biosensor.
研究领域:
材料科学
·
生物传感技术
·
纳米技术
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MATERIALS SCIENCE IN SEMICONDUCTOR PROCESSING
·
2025
·
IF 4.6
Zheng Wu,Changxin Dong,Xinhuan Niu,Jiakai Zhou,Chao He,Xinjie Li,Bin Hu,Jiahui Li
As technology nodes shrink below 10 nm, stricter demands are required for the one-step polishing of copper (Cu) films in ruthenium (Ru)-based Cu interconnects: a high Cu removal rate (RR) and a near-zero Ru RR. In this work, an eco-friendly slurry was newly formulated by combining hydroxyethylethylene diphosphonic acid (HEDP) and phytic acid (PA), both containing phosphate groups, to enhance corrosion inhibition and polishing performance during Cu/Ru CMP. Polishing and electrochemical experiments demonstrated that the synergistic inhibitors achieved a corrosion inhibition efficiency of 96 % for Cu. Under optimized conditions, the material removal rates (MRRs) of Cu and Ru reached 5432 Å/min and 10 Å/min, respectively, with a maximum removal rate selectivity (RRS) of 543:1 and surface roughness ( Sqs ) of 0.76 nm and 0.53 nm. Contact angle, coefficient of friction (COF), Ultraviolet–visible spectroscopy (UV–Vis), X-ray photoelectron spectroscopy (XPS) analyses confirmed the formation of a protective passivation film on Cu/Ru surfaces from both mechanical and chemical perspectives. Theoretical calculations identified the reactive sites of the inhibitors and simulated their adsorption behavior in a CMP environment, revealing that the synergistic inhibitors exhibited the highest adsorption energy. Without the use of surfactants, the multifunctional synergistic inhibitors improved surface quality through lubrication and passivation effects while reducing reagent consumption. This work provides both theoretical and practical guidance for the design of green and efficient CMP slurries in advanced semiconductor manufacturing.
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AICHE JOURNAL
·
2022
·Vol. 68
·期 6
·e17640
·
IF 4.167
Jingpeng Zhang,Yaning Wang,Jiaming Tian,Binhang Yan
Cu-based catalysts, which are regarded as the most promising catalysts for CO 2 conversion, suffer dramatic deactivation at high temperatures. In this work, LaFeO 3 , a typical perovskite-type oxide, is employed to disperse and stabilize Cu particles for the reverse water gas shift reaction. Compared to traditional Cu-based catalysts, Cu/LaFeO 3 exhibits a higher conversion with 100% CO selectivity and better stability at 873 K. Structural and spectroscopic characterization including N 2 O chemisorption, high-resolution transmission electron microscopy, in situ x-ray diffraction, and x-ray absorption fine structure show that metallic Cu is well dispersed on LaFeO 3 , forming more Cu-LaFeO 3 interface. CO 2 temperature-programmed surface reaction (CO 2 -TPSR), two-step transient surface reaction (two-step TSR), and transient in situ diffuse reflectance infrared Fourier transformed spectroscopy experiments demonstrate that the superior activity is attributed to the synergistic effect between the highly dispersed Cu particles for H 2 dissociation and the abundant oxygen vacancies in LaFeO 3 support for CO 2 activation. The synergistic effect between metal and perovskite-type oxide increases metal-support interfaces and enhances CO 2 activation, leading to a potential application in a variety of chemical reactions.
研究领域:
化学工程
·
催化材料科学
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Journal of Cleaner Production
·
2026
·
IF 10.7
Mingyang Zhang,Zihao Chen,Jiehao Zhan,Shaoyong Lu,Yi Chen,Xinshan Song,Hongcan Cui,Chengyu Chen,Lihua Cui,Zhujian Huang
Excessive discharge of copper-containing electroplating wastewater and the widespread misuse of antibiotics pose serious risks to human health and the environment. Herein, an innovative electrochemical closed-loop system was proposed, in which copper-loaded activated carbon fibers (Cu-ACF) were recovered via electrodeposition from Cu-containing wastewater and subsequently employed as cathode to activate peroxymonosulfate (PMS) for doxycycline (DOX) degradation. At an applied potential of −1.1 V, the Cu 2+ deposition capacity reached 729.9 mg⋅g −1 . Copper species were mainly present as Cu 2+ together with Cu 0 /Cu + species on the ACF surface, providing active sites for electron transfer and enhancing PMS activation. Under optimal conditions, more than 95% of DOX was removed within 60 min, exhibiting a pseudo-first-order rate constant about twice that of blank ACF. Cu-ACF 1 also showed good reusability, retaining 85.1% removal efficiency after five cycles. Electrochemical analyses demonstrated that Cu-ACF exhibited enhanced catalytic current response and interfacial activity compared to blank ACF, favoring PMS activation. Multiple reactive oxygen species were identified in the system, with •O 2 − identified as the dominant contributor, while 1 O 2 from a non-radical pathway served as the secondary species. In addition, DOX can be degraded via three pathways, generating 19 intermediate products, most of which exhibit low toxicity. This work provides a sustainable strategy that simultaneously enables copper recovery and efficient antibiotic removal, offering dual benefits for resource recycling and environmental protection.
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ANALYTICA CHIMICA ACTA
·
2026
·
IF 6.1
Chengcheng Qi,Yaqi Kong,Juan Chai,Ziyin Yang
The size effect has a significant impact on the catalytic performance of metal nanostructures, where smaller sizes often correspond to higher specific surface area and specific activity. This study investigates the pyrolysis-temperature-dependent evolution of Cu-MOFs and reveals an anomalous size effect of Cu nanoparticles in glucose electrooxidation. Although low-temperature pyrolysis produces small Cu nanoparticles, the high-temperature pyrolysis product demonstrates exceptional performance despite the larger size of its Cu nanoparticles. The sensor based on larger Cu nanoparticles exhibits 24-fold higher sensitivity compared to small Cu nanoparticles. In-depth study reveals that high-temperature pyrolysis not only produces large-sized Cu nanoparticles but also induces and promotes the formation of oxygen-coordinated Cu single atoms. The coexistence of oxygen-coordinated Cu single atoms electronically modulates adjacent Cu nanoparticles via charge transfer, which accelerates the electron transfer rate and promots the generation of highly active sites at lower operating potentials, thereby overriding conventional size-activity constraints. This study not only highlights the non-negligible role of oxygen-coordinated metal single atoms during high-temperature pyrolysis and provides a new perspective to explain the anomalous size effect, but also redefines sensing materials design principles through single atom-nanoparticle interactions.
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CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Zhi Xu,Zi-He Meng,Song-Hai Wu,Shi-Jie Wang,Peng-Yue Zhu,Yong Liu,Hai-Tao Ren,Shao-Yi Jia,Xu Han
Sulfate radical (SO 4 •− ) is always thought to be an important oxidizing species in the metal-sulfite [S(IV)] systems, however, the oxidizing species correlated with the metal species have rarely been mentioned. In this study, the oxidizing species that oxidize arsenite [As(III)] in the Cu(II)-S(IV) system were investigated under alkaline conditions. Kinetic results indicate that complexation between Cu(II) and S(IV) is the pre-requisite to initiate various oxidizing species, followed by internal electron transfer from S(IV) to Cu(II) with the formation of SO 3 •− and the Cu I (SO 3 ) n −2n+1 complexes. Quenching experiments rule out contributions of SO 5 •− , peroxymonosulfate (HSO 5 − , PMS), hydroxyl radical ( • OH), superoxide radical (O 2 •− ) and singlet oxygen ( 1 O 2 ) to As(III) oxidation in the Cu(II)-S(IV) system and indicate that some kinds of peroxo species contribute. On the other side, apart from the oxidizing species such as SO 5 •− , PMS and SO 4 •− generated via a series of reactions between SO 3 •− and O 2 , the Cu I (SO 3 ) n −2n+1 complexes also react with O 2 to form Cu II -O 2 •− -(SO 3 2− ) n superoxo species and Cu III -O 2 2− -(SO 3 2− ) n peroxo species, as revealed by Raman analysis. UV–vis spectrum further confirms the presence of Cu(III) in the Cu(II)-S(IV) system. We therefore suggest that both SO 4 •− and the Cu(III)-peroxo species play important roles in the oxidation of As(III) in the Cu(II)-S(IV) system. This study enriches our understanding on the diversity of oxidizing species in the metal-S(IV) systems under alkaline conditions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Qiao Yang,Chuanhai Xia,Shuai Chen,Xuezhi Cao,Jingcheng Hao
Hypothesis Despite that the development of Cu 2 SnS 3 (CTS) catalyst has attracted increasing interests, few study has reported to investigate its heterogeneous catalytic degradation of organic pollutants in a Fenton-like process. Furthermore, the influence of Sn components towards Cu (II)/Cu (I) redox cycling in CTS catalytic systems remains a fascinating research. Experiments In this work, a series of CTS catalysts with controlled crystalline phases were prepared via a microwave-assisted pathway and applied in the H 2 O 2 activation for phenol degradation. The efficiency of phenol degradation in CTS-1/H 2 O 2 system (CTS-1: the molar ratio of Sn (copper acetate) and Cu (tin dichloride) is determined to be Sn:Cu = 1:1) was systematically investigated by controlling various reaction parameters including H 2 O 2 dosage, initial pH and reaction temperature. We discovered that Cu 2 SnS 3 exhibited superior catalytic activity to the contrast monometallic Cu or Sn sulfides and Cu (I) acted as the dominant active sites. The higher Cu (I) proportions conduce to the higher catalytic activities of CTS catalysts. Quenching experiments and electron paramagnetic resonance (EPR) further proved that the activation of H 2 O 2 by CTS catalyst produces reactive oxygen species (ROS) and subsequently leads to degradation of the contaminants. A reasonable mechanism of enhanced H 2 O 2 activation in Fenton-like reaction of CTS/H 2 O 2 system was proposed for phenol degradation by investigating the roles of copper, tin and sulfur species. Findings The developed CTS acted as a promising catalyst in Fenton-like oxidation progress for phenol degradation. Importantly, the copper and tin species contribute to a synergetic effect for the promotion of Cu (II)/Cu (I) redox cycle, which thus enhanced the activation of H 2 O 2 . Our work may offer new insight on the facilitation of Cu (II)/Cu (I) redox cycle in Cu-based Fenton-like catalytic systems.
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JOURNAL OF NANOPARTICLE RESEARCH
·
2023
·Vol. 25
·期 8
·1-13
·
IF 2.5
Zhu Jiantao,Wen He,Han Wei,Ma Jiantai,Zhang Feng,Liu Chaowei
The growing concern about the environmental consequences of anthropogenic CO 2 emissions significantly stimulated the research of low-cost, efficient, and recyclable solid adsorbents of CO 2 capture. Metal–organic frameworks (MOFs) are a promising porous material for CO 2 adsorption. Hybrid materials consisting in copper benzene-1,3,5-tricarboxylate (Cu-BTC) and Cu doped graphitic-carbon nitride (Cu-g-C 3 N 4 ) were prepared through solvothermal method as CO 2 adsorbent. The size range of Cu-BTC@1.8%Cu-g-C 3 N 4 was 9.0 ~ 19.4 μm, which was lower than the size range of Cu-BTC (14.6 ~ 29.6 μm). The hybrid adsorbents had lower Brunauer–Emmett–Teller (BET) surface areas and pole volume due to the combination with Cu-g-C 3 N 4 . The CO 2 adsorption capacity of Cu-BTC@1.8%Cu-g-C 3 N 4 increased by 49.5% compared with that of pure Cu-BTC because of more adsorption sites including unsaturated metal centers and N atoms. Moreover, the Cu-BTC@1.8%Cu-g-C 3 N 4 had good stability in CO 2 adsorption capacity after multiple adsorption cycles. Graphical abstract
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Molecular Catalysis
·
2021
·
IF 5.062
Huayan Zheng,Nilesh Narkhede,Guoqiang Zhang,Huacheng Zhang,Lina Ma,Shirui Yu
The small amount of promoter has shown increase in the methanol formation rate by several folds. Hence, hydrotalcite having sufficient trivalent cations are preferred; however, traditional coprecipitation route often leads to poor Cu dispersion owing to higher cationic charge in the layered structure that result in aggregation of the sheets. The present paper reports synthesis of porous, nanostructured Cu/ZnO/Ga 2 O 3 catalysts from pure phase hydrotalcite precursors by using aqueous miscible organic solvent treatment method. The 20% Ga containing catalyst showed ca. 2.5-fold increase in both surface area and % dispersion of the exposed Cu as compared to that prepared from standard coprecipitation method with similar composition. The stabilization induced by mutual dispersion of Cu, Zn and Ga components in the exfoliated sheets resulted in confinement of the Cu particle size up to 5 nm in the spent catalyst. The best performing catalyst of the series, Cu 0.4 Zn 0.4 Ga 0.2 -LDO exhibited STY of 762 mg•g Cat −1 •h −1 for methanol formation from syngas which was decreased by only 8.6% during 50 h of the reaction on stream. Further, it was revealed that, Ga is more conductive to stabilization of Cu as compared to Al, resulting in 23% higher methanol formation rate as compared to the Al containing catalyst.
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