CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Wenyang Fu,Zhongzheng Hu,Yang Zheng,Pei Su,Qizhan Zhang,Yongli Jiao,Minghua Zhou
Compared to traditional haber–bosch process for synthetic ammonia, electrochemical reduction of nitrate to ammonia (ERNA) offers a promising and sustainable technology to generate ammonia at ambient temperature. However, the performance of ERNA is impeded by lacking of sound strategy for designing high-performance electrocatalyst. Here, a Cu based electrode with Cu 2 O/Cu interface was prepared by pulse electrodeposition and electroreduction, achieving the fast rate constant of 0.14 min −1 for reducing nitrate with a high ammonia yield rate of 2.17 mg cm -2 h −1 (faradaic efficiency: 84.36%) and ammonia selectivity of 94.4% at −0.25 V vs. RHE. Particularly, density functional theory (DFT) calculations for the adsorption energy indicated that Cu 2 O/Cu interface alleviated adsorption energy of NO 2 - from −2.02 eV (pure Cu) to −1.59 eV, improving surface diffusion of adsorbed NO 2 - . And DFT calculations for electronic structure implied that Cu 2 O/Cu interface upshifted the d band center of Cu (-2.25 eV vs. −2.48 eV of pure Cu), boosting electron transfer to NO 3 - . Additionally, in-situ infrared spectroscopic analysis confirmed vital intermediates of NO 2 - and NH 2 OH on Cu 2 O/Cu to identify reaction pathway and Gibbs free energy diagram clarified this interface decreased reaction barrier of crucial step (reducing *NO 2 to *NO) from 0.31 eV (pure Cu) to −0.77 eV for the enhancement of ERNA. Thereby, these findings demonstrated that Cu 2 O/Cu interface tunes mobility of NO 2 - and electron transfer to NO 3 - on Cu based electrocatalyst is an efficient method to promote performance of ERNA with high efficiency and rate.
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JOURNAL OF SOLID STATE CHEMISTRY
·
2021
·
IF 3.498
Ping-Ping Sun,Yu-Hang Zhang,Hongwei Shi,Fa-Nian Shi
A new 3-D Co-MOF with the molecular formula of C 10 H 8 Co 3 N 4 O 12 was prepared by hydrothermal method . As the anode for lithium ion battery , the electrode modified with 20% copper powder (Co-MOF-20) shows the specific capacity of 1138.5 mAh g −1 at 100 mA g −1 . Even under the high current test of 500 mA g −1 , Co-MOF-20 also shown excellent performance (349.6 mAh g −1 ) after 300 cycles. The advantages of Co-MOF-20 electrode are not only due to the introduction of copper powder conductive agent, but also the existence of three-dimensional structure which can provide ion transport channels.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Yiping Guo,Wei Xie,He Li,Jianping Li,Jun Hu,Honglai Liu
The adsorption desulfurization (ADS) is a promising technology for deep removing thiophene-type sulfurs, yet it remains challenges in maintaining good performance for real applications in the presence of water. Guided by theoretical calculations, we constructed hydrophobic selective channels by crosslinking porous aromatic framework (PAF) of PAF-56 on the surface of adsorbent MOF-199 with Cu nodes reduced. The optimized Cu(I)-BTC@PAF30 shows a high saturated dibenzothiophenes (DBT) adsorption capacity of 61.7 mgS g −1 from the dehydrated model oil. Attributed to the good DBT-affinity (with binding energy (BE) of −90.52 KJ mol −1 ) and water-repulsion (with BE of −14.72 KJ mol −1 ), PAF-56 coating layer significantly improves the hydrophobicity , and keeps the DBT adsorption capacity as high as 50.8 mgS g −1 in the presence of 0.5% (v/v) water, the decline of 17.6% was much smaller than the dramatical 70.9% decrease in pristine Cu(I)-BTC. More importantly, it effectively prevents Cu(I) nodes from the oxidation , and exhibits a superior stable cyclic performance with the removal efficiency above 91% after 20 cycles. Therefore, Cu(I)-BTC@PAF30 can be a good representative of this surface modification strategy to achieve promising application in industrial ADS.
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FUEL
·
2023
·
IF 7.4
Yanqing Shi,Cai Guo,Huajing Zhou,Liang He,Shaoyun Shan,Tianding Hu
Rational modulation of the local electron density of Cu active site is the key to improve the efficient transfer hydrogenation (CTH) of furfural (FF) on the surface of catalysts with low Cu-loadings. In this paper, a CuMgAl/LSC catalyst with lower Cu content (<3.5 % wt ) was prepared by using porous biochar as a carrier and exploiting the local dispersion and electron-modulation effects of structural elements of hydrotalcite laminates. CTH experiments showed that the conversion of FF and the selectivity of FA could reach more than 99.0 % in isopropanol solution at 170 °C and within 1 h. Catalyst characterization and density functional theory (DFT) calculations demonstrated that the Cu(I) species was the main active site during the CTH process of FF. Doping laminate metals (i.e., Mg, Al) can not only form electron-rich centers by local electron modulation of the active site through the coordination structure of Cu-O-M, lowering its D-band center and achieving higher catalytic activity; Due to the Jahn-Teller effect, the local spatial misalignment of Cu sites formed, which can reduce the risk of over-hydrogenation and improve the FA selectivity. In addition, it can be also found that the Coulomb tractive force of reactive intermediates can lead to the crystal surface reconstruction and structure deterioration of Cu species. The new discovery of the deactivation mechanism can provide a reference for the future design of copper-based catalysts in CTH process of FF.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2022
·
IF 6.76
Yizhen Yu,Bingzhi Li,Yinsha Wei,Xinyue Ren,Fengsai Bie,Yang Xu,Ri Qiu,Xiaoguang Li,Yibo Ouyang
In the harsh environment, the corrosion of Cu leads to the failure of pipelines, condenser, printed circuit board and so forth. Thus, protecting Cu from corrosion is critically important from both science and engineering backgrounds. In this report, the hierarchical structure compositing dendritic Cu and ZIF-67 is prepared onto Cu by a two-step electrodeposition protocol. After thiol modification and oil infusion, bio-inspired superhydrophobic surface (SHS) and slippery liquid-infused porous surface (SLIPS) is respectively achieved, and sophisticated techniques are used for characterizing chemical composition, morphology, topology and wettability. Scanning Kelvin probe is employed to know the surface potential distribution before and after the biomimetic transformation. Using different electrochemical approaches, the corrosion inhibition effect is elucidated. In 3.5 wt% NaCl corrosive medium, |Z| 0.01Hz of SLIPS is as high as 1.35 × 10 8 Ω·cm 2 at the initial immersion stage. The value is remarkably enhanced compared with SHS (6.76 × 10 4 Ω·cm 2 ) and bare Cu (8.74 × 10 3 Ω·cm 2 ). After soaking for 168 h, |Z| 0.01Hz value of SHS and SLIPS is 3.84 × 10 4 Ω·cm 2 and 4.93 × 10 6 Ω·cm 2 , illustrating that SLIPS has high resistance to protect Cu from corrosion.
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Nanomaterials
·
2023
·Vol. 13
·期 13
·1897
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IF 5.3
Bairui Qi,Qiang Xu,Yunxuan Cao,Zhu Xiao
Copper and iron are the basic metal elements that have attracted much attention in industry. Prussian blue (PB) is a significant class of metal–organic frameworks (MOFs); however, the lack of such linkages between the structure and properties, as well as properties differences, limits their potential applications. In this paper, the Cu-based Prussian blue nanocubes with and without Fe doping were synthesized. With the increasing reaction time, the morphology of the Cu-based Prussian blue nanocubes without Fe doping (PB:Cu NCs) changes from cuboidal to circular, and finally grows back to cuboidal. However, Cu-based Prussian blue nanocubes with Fe doping (PB: CuFe NCs) grow directly from the cube and eventually collapse. The nanocubes show a notable red shift with the tunable spectra from 400 nm to 700 nm. Compared with PB: Cu NCs, the PB: CuFe NCs have higher temperature rise under 808 nm irradiation and better photothermal efficacy. The catalytic efficiency of PB: CuFe NCs changes with the pH and reaches its maximum value of 1.021 mM with a pH of 5.5. The enhanced catalytic reaction by the near-infrared radiation plasmonic photothermal effect is also confirmed. This work highlights the potential of the developed PB: Cu and PB: CuFe NCs for photothermal-enhanced co-catalysis nanomaterials.Keywords:Prussian blue;photothermal effects;catalytic reaction;synergistic action;copper
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JOURNAL OF NANOBIOTECHNOLOGY
·
2026
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IF 15
Xie Wenjie,Xu Qianfeng,Yao YueXian,Chen Muqi,Zou Fen,Lin Jundong,Zhong Guowei,Zhou Haoran,Xu Jiaquan,Luo Pu,Liang Zhenguo,Du Qiuling,Li Jibiao,Zhang Jinxiang,Lu Puyang,Zhang Yixun,He Huichan,Zhuo Yangjia,Zhong Weide
Prostate cancer (PCa) is the most prevalent malignant tumor in the male genitourinary system. Carbon monoxide (CO) gas therapy and chemodynamic therapy (CDT) have emerged as alternative treatments for cancer. However, the therapeutic efficacy of both approaches is constrained by the insufficient endogenous hydrogen peroxide (H 2 O 2 ) supply and the overexpression of protective glutathione (GSH) in the tumor microenvironment (TME). Herein, we developed a biomimetic cascaded nanoreactor (DCM@MCuH@MnCO) for synergistically combining CO-mediated gas therapy with CDT driven by depletion of GSH and self-supply of H 2 O 2 in the tumor. DCM@MCuH@MnCO was constructed by integrating a copper-catechol coordinated network (CuH) and H 2 O 2 -sensitive manganese carbonyl (MnCO) within the mesoporous carbon hollow spheres (MCHS), and further modifying the surface with tumor cell membranes (DCM) to enhance its tumor-targeting ability. The CuH in the nanoreactor can disassemble, triggered by continuous consumption of GSH, releasing pro-oxidative catechol ligands to generate H 2 O 2 for TME remodeling. Subsequently, MnCO decomposes on demand to release CO in situ while copper ions (Cu + ) convert H 2 O 2 into reactive oxygen species (ROS) via a Fenton-like reaction. These events cooperatively cause mitochondrial damage and induce a lethal ROS storm within cells, ultimately effectively killing tumor cells both in vitro and in vivo. This study demonstrates significant prospects for CO therapy and CDT, offering a novel and promising strategy for efficient PCa treatment. Graphical
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CATALYSIS LETTERS
·
2026
·Vol. 156
·期 10
·282
·
IF 2.5
Ye Qihang,Zhong Zhaoping,Yang Yuxuan,Wang Wei,Jia You,Xiong Qi,Chen Huanqi,Zheng Xiang
Furfural, a key biomass-derived platform chemical, requires efficient hydrogenation for economic and research benefits. Herein, we propose a carbon-encapsulated catalyst with optimized active sites (using carbon-containing organics) for its highly selective hydrogenation. Experimental results demonstrated that carbon loading facilitated the conversion of strong acid sites to medium‑strong acid sites on the catalyst support, and also increased the Lewis/Brønsted (L/B) ratio. Through optimization of reaction conditions and carbon loading, complete conversion of furfural and a furfuryl alcohol selectivity as high as 99.17% were achieved at 160 °C for 4 h. The prepared catalyst maintained high furfuryl alcohol selectivity even after five cycles, owing to the protective carbon layer on the active support and the well-dispersed Cu species on its surface. DFT calculations further revealed that furfural preferentially adsorbs on the catalyst surface via the η¹(O)-aldehyde configuration, confirming the promotional role of the catalyst in furfural hydrogenation. Graphical
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Jiahao Zhu,Jianqing Ma,Sijing Yao,Mika Erik Tapio Sillanpää,Minghua Zhou,Chensi Shen,Qing Ye,Huixia Jin,Kefeng Zhang
Heterogeneous Fenton-like systems using H 2 O 2 as an oxidant have been extensively investigated in acidic and neutral conditions, but usually, they become ineffective under alkaline conditions. In this study, a cuprous graphitic carbon nitride material (Cu–CN) was prepared that can generate singlet oxygen ( 1 O 2 ) from H 2 O 2 . The results demonstrate that at pH 11, 95 % of 50 mg/L p -chlorophenol (4-CP) can be effectively eliminated within 120 min. Through semi-quantitative analysis and density functional theory calculations, it has been confirmed that 1 O 2 is the dominant reactive oxygen species in this system under alkaline conditions. The main pathway for 1 O 2 generation involves the formation of a complex between · O 2 – and Cu(II)-N sites, and the subsequent intramolecular electron transfer. To enhance the stability and separation performance of this catalyst, polyethylene glycol (PEG) was employed as a binder to combine Cu–CN with Fe 3 O 4 . The terminal hydroxyl groups in PEG were cross-liked by metals, thus forming a solid and magnetic composite (CuFe@PEG). Compared to Cu–CN, CuFe@PEG exhibited remarkable performance with 93 % retention of its original capacity for 4-CP removal at pH 11. Furthermore, after seven cycles, the degradation efficiency only decreased by 6.36 %. This study introduces a novel approach for utilizing Fenton-like reactions in treating alkaline wastewater.
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DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 47
·17981-17992
·
IF 4
Changzhen Wang,Xueqing Hai,Jia Li,Yupeng Liu,Xiaosheng Yu,Yongxiang Zhao
We studied the Ni–Cu-acid multifunctional synergism in NiCu-phyllosilicate catalysts toward 1,4-butynediol hydrogenation to 1,4-butanediol by varying the reduction temperature, which can activate different bimetal and support interactions. Compared with a monometallic Ni phyllosilicate (phy), which only showed one type of metal species when reduced at ∼750 °C, there are three types of metal species for the bimetallic Ni–Cu-phyllosilicate derived catalysts, namely Cuphy, differentiated Ni, and Niphy. Thorough structure–activity/selectivity correlation investigations showed that, although the Ni9Cu1-P catalyst matrix can produce tiny amounts of differentiated Ni0 species under the induction of reduced Cu0 at R250 condition, it could not form Ni–Cu bimetallic interactions for the collaborative hydrogenation of 1,4-butynediol, and the product stays in the semi hydrogenated state. When the reduction temperature is raised to 500 °C, stable Ni–Cu alloy active sites exist, accompanied by the strong metal support interaction and metal acid effect derived from the intimate contact between the extracted metal sites and the surviving functional phyllosilicate support; these functionalities yield a supreme hydrogenation performance of the R500 sample with a 1,4-butanediol yield larger than 91.2%.
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Advanced Healthcare Materials
·
2023
·
IF 10
Lin Zhang,Jin-Mei Fu,Lai-Bo Song,Kai Cheng,Fang Zhang,Wen-Hui Tan,Jin-Xuan Fan,Yuan-Di Zhao
Multi-modal combination therapy for tumor is expected to have superior therapeutic effect compared with monotherapy. In this study, a super-small bismuth/copper-gallic acid coordination polymer nanoparticle (BCN) protected by polyvinylpyrrolidone is designed, which is co-encapsulated with glucose oxidase (GOX) by phospholipid to obtain nanoprobe BCGN@L. It shows that BCN has an average size of 1.8 ± 0.7 nm, and photothermal conversion of BCGN@L is 31.35% for photothermal imaging and photothermal therapy (PTT). During the treatment process of 4T1 tumor-bearing nude mice, GOX catalyzes glucose in the tumor to generate gluconic acid and hydrogen peroxide (H 2 O 2 ), which reacts with copper ions (Cu 2+ ) to produce toxic hydroxyl radicals (•OH) for chemodynamic therapy (CDT) and new fresh oxygen (O 2 ) to supply to GOX for further catalysis, preventing tumor hypoxia. These reactions increase glucose depletion for starvation therapy , decrease heat shock protein expression, and enhance tumor sensitivity to low-temperature PTT. The in vitro and in vivo results demonstrate that the combination of CDT with other treatments produces excellent tumor growth inhibition. Blood biochemistry and histology analysis suggests that the nanoprobe has negligible toxicity. All the positive results reveal that the nanoprobe can be a promising approach for incorporation into multi-modal anticancer therapy.
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FOOD CHEMISTRY
·
2023
·
IF 8.8
Liqin Kong,Feng Hong,Peng Luan,Yiping Chen,Yaoze Feng,Ming Zhu
The development of biosensors capable of assessing umami intensity has elicited significant attention. However, the detection range of these biosensors is constrained by the sensing components and strategies used. In this study, we introduce a novel competitive, ultra-high-sensitivity electrochemical impedance biosensor by utilizing composite nanomaterials and T1R1 as a composite signal probe. Pd/Cu-TCPP(Fe) had a substantial surface area, effectively enhancing the loading capacity of the T1R1 and thus augmenting the biosensor's recognition precision. Furthermore, the Pd/Cu-TCPP(Fe) elevated peroxidase-like activity catalyzed the formation of insoluble precipitates of 4-CN, resulting in cascaded amplification of the impedance signal. The remarkable catalytic activity of the composite signal probe endowed the biosensor with exceptional analytical performance, featuring a detection limit of 0.86 pg/mL and a linear detection range spanning from 10 to 10000 pg/mL. Successful application of the biosensor for umami substance detection in fish was also demonstrated, signifying its substantial potential in food-flavor evaluation.
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