ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Qichen Wang,Jun Li,Qiuying Wang,Haotian Tan,Yunrui Tian,Chao Wang,Wenping Si,Yangsen Xu,Xiao Yan,Ji Liang
Electrocatalytic ammonia oxidation reaction (AOR), as a promising energy conversion technology, also offers ideas for the synthesis of high-value nitrogenous compounds such as nitrites and nitrates. However, the sluggish kinetics of AOR at the anode leads to high overpotential and elevated energy consumption, necessitating advanced catalysts. Here, we engineer a NiO/CuO heterojunction on a copper mesh (NiO/CuO@Cu), which generates a robust internal electric field at the NiO–CuO interface. The built-in electric field facilitates interface electron redistribution and surface electronic state modulation, significantly enhancing the charge transfer and AOR kinetics. The NiO/CuO@Cu catalyst exhibits a low onset potential of 1.38 V vs RHE, along with 95.8% ammonia conversion efficiency and 90.6% nitrite selectivity during 8-h operation at 1.6 V vs RHE. Notably, the catalyst shows excellent operation stability for over 56 h. This work presents interface engineering through heterojunction design as an effective strategy for AOR enhancement, providing valuable insights for developing high-performance electrocatalysts in energy conversion technologies.
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高影响因子
MOLECULES
·
2022
·Vol. 27
·期 20
·7064
·
IF 4.927
Jia Liu,Chao Ding,Sicheng Gong,Kun Fu,Huiping Deng,Jun Shi
The nonradical process in the peroxydisulfate (PDS) oxidation system is a promising method for antibiotic removal in water. In this study, CuO@CNT was successfully synthesized by a facile approach to catalyze PDS. The removal efficiency of the antibiotic sulfamethoxazole (SMX) was 90.6% in 50 min, and the stoichiometric efficiency (ΔSMX/ΔPDS) was 0.402. The very different degradation efficiency of common organic contaminants revealed the selective oxidation of the surveyed system. The process of1O2oxidation and the electron-transfer regime was exhibited by chemical quenching tests, electron paramagnetic resonance (EPR) determination, a UV–vis spectrophotometer, X-ray photoelectron spectroscopy (XPS) detection, and cyclic voltammetry (CV) measurements. Sustainable catalysis was promoted by the circulation between the surface electron-rich centers of Cu(II) and Cu(III). Dissolved oxygen (DO) and a metastable Cu(III) intermediate contributed to the generation of1O2. Still, a portion of SMX was removed by the mildly activated PDS. Moreover, the influence factors (pH, dosage, water matrix) were examined, and suppressions were acceptable by common anions and real water. Distinguished from the radical process, unique intermediate products were ascertained via the theoretical calculation and liquid chromatography–mass spectrometry (LC-MS) detection. Furthermore, CuO@CNT showed a satisfactory activation ability in the cycling experiments. Overall, this study developed CNT to be a supporter of CuO, unveiled the mechanism of catalysis, and evaluated the application potential of the nonradical process.Keywords:peroxydisulfate;nonradical process;singlet oxygen;trivalent copper;electron transfer
研究领域:
环境科学
·
化学
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
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IF 3.498
Longlong Geng,Gang Li,Xiuling Zhang,Xiangmei Wang,Chunhui Li,Zhongmin Liu,Da-Shuai Zhang,Yong-Zheng Zhang,Guangyin Wang,Haixiang Han
Morphology and surface property are critical property-defining factors for metal oxide catalysts, therefore, the rational engineering on these aspects is considered as the effective means to enhance their overall catalytic activities. In this work, a silicon oxide (SiO 2 ) with hierarchical structure was successfully prepared and applied as carrier for the design of SiO 2 -supported copper oxide catalysts (CuO/SiO 2 -x, x represents treating temperature of SiO 2 during preparation). The morphology and composition of thus-obtained catalysts were characterized by XRD , SEM, HRTEM , XPS , FTIR , contact angle and N 2 adsorption. Interestingly, even with relatively large CuO particles , excellent activity was also achieved in hydrogenation of nitrophenol under relatively mild conditions (25 °C and 1 atm). Over the optimal CuO/SiO 2 -800 catalyst, the 4-nitrophenol (4-NP) conversion reached 99% in 60 s and its hydrogenation rate was about 9.2 times that of bare CuO catalyst. Additionally, it could also be reused for at least eight times without obvious fading in efficiency. The excellent catalytic performance can be attributed to the synergy between surface-anchored structure in which more active sites can be exposed, and hydrophilic surface to promote the adsorption and diffusion of substrate molecules during hydrogenation process.
研究领域:
催化化学
·
材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2026
·
IF 9.6
Xingxin Pan,Xize Chen,Yuwen Liu,Min Wang,Yujia Liu,Hongyu Zhang,Liang Feng
The engineering of the nanozyme interface is crucial for manipulating their catalytic efficacy, yet achieving this through chirality modulation still remains a significant challenge. In this work, a chirality-driven interface engineering strategy by constructing chiral L/D‑copper oxide hierarchical architectures (L/D-CuO) via a facile one-step wet-chemistry method using enantiomeric cysteine ligands. The resulting hierarchical architectures feature flower-like architectures, and more importantly exhibit intense and chiroptical activity, unambiguously confirming the successful creation of a tailored chiral interface. Steady-state kinetic analyses revealed that the engineered chiral interface significantly augmented the peroxidase-like (POD-like) activity. The L-CuO demonstrated a lower Michaelis-Menten constant (Km = 1.003 mM) and a higher maximal reaction rate (Vm = 0.0252 μM·s −1 ) compared to achiral CuO (Km = 1.38 mM, Vm = 0.0185 μM·s −1 ), indicating enhanced substrate affinity and catalytic efficiency at the interface. This augmented interfacial catalysis was effectively translated into potent antibacterial action. The L-CuO achieved a bacterial inhibition rate reaching 90.2% against E. coli and 93.1% against S. aureus , compared with only 59.3% for E. coli and 66.9% for S. aureus antibacterial efficacy for achiral CuO. In practical fruit preservation, the chiral hierarchical architectures effectively functioned as an interfacial antimicrobial coating, significantly preserving fruit quality by inhibiting surface microbial spoilage. This work highlights the profound impact of chirality-driven interface engineering on nanozyme functionality and provides a foundational strategy for designing advanced interfacial catalysts for antibacterial and other biomedical applications.
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APPLIED SURFACE SCIENCE
·
2023
·
IF 6.7
Mingji Xu,Xi Ran,Ruoli Chen,Maoshen Chen,Ruijuan Qi,Chengqin Dai,Chunhua Luo,Hui Peng,Hechun Lin
Gas sensors based on metal/metal oxide heterostructures have shown rapid advancements due to their excellent sensing performance. However, it is difficult to control the formation of Cu/CuO nanostructure due to the easy oxidation of copper and limits its sensing application. Herein, we reported the controlled oxidation of Cu superfine particles (SPs) to form Cu/CuO nanostructure via reducing CuO with monoethanolamine, oxidized with H 2 O 2 and then in-situ annealed at 250 °C. The organic residue generated during the reducing step plays a key role in controlling the oxidation of Cu SPs to form Cu/CuO nanostructure. The nanomaterial was used to fabricate gas sensor, which presents excellent p-type sensing performance to ethanol with good selectivity and a good linear relationship in the range of 1 to 100 ppm ethanol. The response to 100 ppm ethanol can be up to 99.40 under 200 °C operating temperature, and the response under 250 °C is 30.66 with the shorter response and recovery time of 214 s and 74 s, respectively. The sensing mechanism can be explained by the adsorption–desorption model. This study provides a promising strategy for the synthesis of Cu/CuO nanostructure and open a new avenue for the development of highly sensitive ethanol sensor.
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Catalysts
·
2022
·Vol. 12
·期 1
·104
·
IF 4.501
Ying Duan,Qianqian Luo,Renfeng Nie,Jianshe Wang,Yongsheng Zhang,Tianliang Lu,Chunbao Xu
The production of methyl lactate as a degradable polymer monomer from biomass was an important topic for a sustainable society. In this manuscript, glycerol was oxidated to methyl lactate catalyzed by the combination of Au-CuO and Sn-Beta. The influence of Sn content, Sn source, and the preparation conditions for Sn-β was studied. The Au content in Au/CuO was also investigated by varying the Au content in Au/CuO. The catalysts were characterized by XRD, FTIR spectroscopy of pyridine adsorption, and TEM to study the role of Sn and the influence of different parameters for catalyst preparation. After the optimization of reaction parameters, the yield of methyl lactate from glycerol reached 59% at 363 K after reacting in 1.6 MPa of O2for 6 h.Keywords:glycerol;oxidation;methyl lactate;Sn-Beta;Au/CuO
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Peng Xu,Peng Wang,Xiang Li,Rui Wei,Xiaojing Wang,Chunyan Yang,Tianyao Shen,Tong Zheng,Guangshan Zhang
CuO-Fe 2 O 3 /MXene was fabricated using a rapid microwave hydrothermal method and used for the enhanced peroxymonosulfate (PMS) activation and atrazine (ATZ) degradation. The ATZ degradation rate could reach up to nearly 100% within 60 min at pH = 6.4, with low dosage for CuO-Fe 2 O 3 /5% MXene (0.1 g‧L -1 ) and PMS (0.37 mM). Experimental results and DFT calculations showed that coexisting matter had little influence on ATZ degradation at low concentrations, indicating the excellent anti-interference capability of the system. Circulation and interaction of ≡Fe(III)/≡Fe(II) and ≡Cu(II)/≡Cu(I) produced SO 4 •- and •OH, O* and SO 5 •- could participate in the formation of 1 O 2 . Then, ATZ degradation pathways, including dealkylation, dichlorination-hydroxylation, alkyl hydroxylation, alkyl oxidation, olefination, and deamination-hydroxylation processes, were proposed based on DFT calculations and ESI-QTOF-MS/MS data. QSAR analysis illustrated that most intermediates were more environmentally friendly than ATZ. This study developed novel materials with superior catalytic performance for elimination of refractory organic pollutants in wastewater.
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COMBUSTION AND FLAME
·
2022
·
IF 5.767
Lyu Jie-Yao,Yang Su-Lan,Wu Shixi,Tang Gen,Yang Wenming,Yan Qi-Long
Burning rate modulation is a critical but challenging technology for solid propellants’ design. Great efforts have been made to synthesize and utilize catalysts to modify the pressure exponent ( n ), but poor catalytic efficiency and lower energy level of conventional catalysts limit their further applications. In this research, interfacial control of Al@AP together with precise catalysis of CuO is represented for the purpose of pressure exponent reduction and combustion performance improvement. The core-shell structured Al@AP and Al@AP/CuO composites were prepared and applied into HTPB/Al/AP composite propellants. These prepared propellants have the same formula but different micro-structures of ingredients, leading to varied combustion performance, in terms of the burning rates, combustion wave structures, flame spectra, agglomeration processes of Al particles and condensed combustion products . The investigation results show that by using interfacial control of Al@AP and precise catalysis of CuO, the n of involved propellants over 1–4 MPa can be greatly decreased from 0.42 to 0.21 and the agglomeration of Al could be effectively inhibited. In addition, propellants based on Al@AP and Al@AP/CuO interfacial controls of this research are summarized and compared together with those based on Al@RDX published recently, to present overall characteristics of interfacial control techniques, which could lead to the development of new smart controllable propellants.
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CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2022
·Vol. 38
·期 4
·919-927
·
IF 2.726
Zhu Junlun,Cui Qian,Wen Wei,Zhang Xiuhua,Wang Shengfu
Although great progress has been made in the advancement of nanozymes, most of the studies focus on mimicking peroxidase, oxidase, and catalase, while relatively few studies are used to mimic laccase. However, the use of nanomaterials to mimic laccase activity will have great potential in environmental and industrial catalysis. Herein, Cu/CuO-graphene foam with laccase-like activity was designed for the identification of phenolic compounds and the detection of epinephrine. In a typical experiment, the formation mechanism of Cu/CuO-graphene foam was investigated during the pyrolysis process by thermogravimetric-mass spectrometry. As a laccase mimic, Cu/CuO-graphene foam exhibited excellent catalytic activity with a Michaelis-Menten constant and a maximum initial velocity of 0.17 mmol/L and 0.012 µmol·L −1 ·s −1 , respectively. Based on this principle, Cu/CuO-graphene foam nanozyme could differentially catalyze phenolic compounds and 4-aminoantipyrine for simultaneous identification of phenolic compounds. Furthermore, a colorimetric sensing platform was fabricated for the quantitative determination of epinephrine, showing linear responses to epinephrine in the range of 3 µg/mL to 20 µg/mL with the detection limit of 0.2 µg/mL. The proposed Cu/CuO-graphene foam nanozyme could be applied for the identification of phenolic compounds and the detection of epinephrine, showing great potential applications for environmental monitoring, biomedical sensing, and food detection fields.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Tao Zhou,Yi Han,Wei Xiang,Chen Wang,Xiaohui Wu,Juan Mao,Mingjie Huang
Heterogeneous catalytic activation mechanisms of peroxydisulfate (PDS) by transition metal oxides are generally attributed to the interactions between catalysts and PDS, however, the role of the co-existed organic substrate was largely overlooked in the past studies. In this work, phenol was selected as the target organic pollutant in a CuO/PDS system to evaluate its deep-seated role in participating in the effective activation of PDS. First, optimized reaction conditions as pH of 6.0, CuO of 5.96 g·L −1 and PDS of 2.5 mM were obtained by the response surface methodology (RSM) with a phenol degradation efficiency of 84.0%. It was further found that pre-adsorption of phenol or PDS led to obviously different performances in the phenol degradation with/without the radical scavengers. Two different activation pathways of PDS, i.e., the non-radical pathway mediated by surface deprotonated phenol to generate 1 O 2 and the radical pathway mediated by structural Cu(I)/Cu(II) to produce SO 4 − , were therefore proposed, and the former was predominant in the CuO/PDS/phenol system. In addition, HCO 3 − and HPO 4 2− could strongly inhibit the phenol degradation while Cl − and NO 3 − only performed negligible effects. NaOH washing could regenerate the surface hydroxyl groups and recover the catalytic ability of CuO. The result of this study integrated the interactions among the catalyst, oxidant and substrate, providing new insights into environmental-friendly PDS activation processes.
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RSC Advances
·
2021
·Vol. 11
·期 21
·12532-12542
·
IF 3.361
HanShuang Liu,KaiJun Wang,XiaoYan Cao,JiaXin Su,Zhenggui Gu
In this study, different magnesium, copper, lanthanide single metal, and composite multimetal oxide catalysts were prepared via the coprecipitation route for the aerobic oxidation of cumene into cumene hydroperoxide. All catalysts were characterized using several analytical techniques, including XRD, SEM, EDS, FT-IR, BET, CO2-TPD, XPS, and TG-DTG. La2O3–CuO–MgO shows higher oxidation activity and yield than other catalysts. The results of XRD and SEM studies show that the copper and magnesium particles in the catalyst are smaller in size and have a distribution over a larger area due to the introduction of the lanthanum element. The CO2-TPD results confirmed that the catalyst has more alkali density and alkali strength, which can excite active sites and prevent the decomposition of cumene hydroperoxide. XPS results show that due to the promotional effect of La2O3, there are more lattice and active oxygen species in the catalyst, which can effectively utilize the lattice defects under the strong interaction between metal oxides for rapid adsorption and activation, thus improving the oxidation performance. Besides, La2O3–CuO–MgO exhibits good stability and crystalline structure due to its high oxygen mobility inhibiting coking during the cycle stability test. Finally, the possible reaction pathway and promotional mechanism on La2O3–CuO–MgO in cumene oxidation are proposed. We expect this study to shed more light on the nature of the surface-active site(s) of La2O3–CuO–MgO catalyst for cumene oxidation and the development of heterogeneous catalysts with high activity in a wide range of applications.
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ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Jun Wang,Bin Li,Yang Li,Xiaobin Fan,Fengbao Zhang,Guoliang Zhang,Yuanzhi Zhu,Wenchao Peng
In this work, γ-Al2O3-supported CuO (c-CuO/Al2O3) materials are successfully synthesized using a novel impregnation–precipitation–decomposition method. The obtained c-CuO/Al2O3 catalyst shows excellent catalytic activities for bisphenol A (BPA) degradation with sodium persulfate (PDS) as an oxidant. Radical quenching tests and electron paramagnetic resonance (EPR) studies indicate that PDS activation is a combined mechanism involving both free radical and nonfree radical pathways. In a continuous large-scale degradation process, about 1.78 L of 20 ppm BPA can be completely removed within 480 min. Although c-CuO/Al2O3 can be deactivated after several reaction cycles, the catalytic activity can be regenerated after simple aerobic calcination. X-ray photoelectron spectroscopy (XPS) and Raman analysis confirm that the deactivation of c-CuO/Al2O3 should be attributed to the conversion of Cu(II) to Cu(I). The aerobic calcination could oxidize Cu(I) back to Cu(II), thus recovering the catalytic activity. In addition, the density functional technology (DFT) and temperature-programmed oxidation (TPD) results reveal that γ-Al2O3 can not only serve as a carrier to anchor the CuO particles but also can adsorb and activate PDS by introducing more basic sites on the surface. c-CuO/Al2O3 has high activity and can be regenerated easily, thus having great potential applications for wastewater treatment.
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