GREEN CHEMISTRY
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2025
·
IF 9.2
Kaiwei Meng,Ziyi Fan,Huiming Wen,Yujie Hu,Wenjun Zhang,Zupeng Chen
The electrochemical conversion of glycerol-a biodiesel byproduct into formic acid coupled with hydrogen evolution reaction (HER) offers a green route for biomass utilization. However, existing systems suffer from high energy demands and insufficient selectivity. Herein, a self-grown copper oxide nanorods decorated with platinum species (Pt/CuO NRs) is developed, reaching a current density of 20 mA cm-2 at 1.14 V vs. RHE, with 97.4% formic acid selectivity at 1.40 V vs. RHE and nearly 100% glycerol conversion. Electrochemical impedance spectroscopy and in situ Raman spectroscopy reveal that Pt0 sites enhance electron transfer at the Cu3+-OH-Pt interface, facilitating CuⅢ-OOH formation. Density functional theory (DFT) analysis shows that Pt weakens O-H bond strength in CuOOH and lowers the dehydrogenation energy barrier, synergistically boosting GOR. Furthermore, a membrane electrode assembly (MEA) with Pt/CuO NRs as the anode and Pt/CuOx (c-Pt/CuOx) as the cathode is established for GOR and HER, respectively, which can operate at 1.55 V for a current density of 100 mA cm-2, reducing the potential by 380 mV compared to water splitting. The developed GOR(+)||HER(-) electrolyzer demonstrates stable performance for 100 hours at 150 mA cm-2, with a formic acid selectivity of 90%. This represents a significant improvement over existing copper-based catalysts, highlighting the green chemistry advantages. The techno-economic analysis demonstrated the economic viability of electrochemically converting glycerol into potassium dicarboxylate (KDF) and H₂, with processing costs of $4655-4797 per ton and a market value of $6389 per ton at representative commercial current densities of 100 and 300 mA cm-2.
研究领域:
化学工程
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材料科学
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能源技术
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DOI
高影响因子
Nature Communications
·
2025
·Vol. 16
·期 1
·1-15
·
IF 15.7
Yue Yuxue,Yu Mingde,Yao Zhangyi,Fang Guangzong,Wang Bolin,Wang Saisai,Jin Chunxiao,Chang Renqin,Sun Tulai,Pan Zhiyan,Zhu Yihan,Wang Feng Ryan,Li Xiaonian,Zhao Jia
Achieving specific orbital activation of C ≡ C by controlling the precise atomic architecture of supported metals is crucial for the selective transformation of alkynes. However, its physical mechanism remains a subject of debate. Herein, we construct a well-defined O-bridged CuN 3 -O-CuN 3 integrative catalytic pairs (Cu ICPs) based on Kirkendall effect. As a result, Cu ICPs with mixed Cu 2+ -Cu 3+ species demonstrate >99% conversion and >550 h stability in acetylene hydrochlorination (simulated industrial reaction conditions), showcasing unparalleled performance in the liquid-phase hydrochlorination of five alkynes as well. A combined experimental and theoretical analyses reveal selective coupling between the d xz / d yz orbitals of Cu ICPs and the σ orbitals of C ≡ C in C 2 H 2 , leading to the formation of highly reactive di- σ -HC = CH intermediate. Additionally, the presence of the bridged-O species promotes HCl dissociation, altering the addition pathway from the classical Eley-Rideal (E-R) mechanism to a Cl•-trigged Langmuir-Hinshelwood (L-H) mechanism, ultimately reducing the intrinsic energy barrier for addition, and breaking the universal standard electrode potential linear scaling relations.
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PubMed
高影响因子
Analytical Methods
·
2022
·Vol. 14
·期 39
·3911-3920
·
IF 3.532
Limin Yang,Xiaolong Zhang,Mingming Li,Linjiao Qu,Zhen Liu
Immobilization of enzymes is one of the key steps in the development of high-performance enzymatic electrochemical biosensors, and various nanostructured materials have been designed and developed to achieve this goal. Herein, hybrid nanoflowers (HNFs) were synthesized using acetylcholinesterase (AChE) as an organic component and copper phosphate (Cu3(PO4)2) as an inorganic component. These AChE–Cu3(PO4)2 HNFs exhibit a three-dimensional hierarchical flower-like structure, which not only has a large specific surface area but also promotes the affinity between AChE and its substrate with better catalytic activity. Not only that, the surface modification of the glassy carbon electrode (GCE) by the joint use of gold nanoparticles (AuNPs) and graphene oxide (GO) extended the electroactive area. Using square-wave voltammetry (SWV), the as-prepared biosensor (i.e., AChE–Cu3(PO4)2 HNF/AuNP/GO/GCE) demonstrated superior sensing performance in the detection of dichlorvos. The detection limit is as low as 0.07 pM, and the linear detection range can range from 0.5 pM to 10 μM. In addition, the biosensor was feasible in real agricultural samples with satisfactory recoveries (98.65% to 103.43%). The reported biosensor provides an alternative tool for the direct measurements of AChE activity and its inhibition. Besides organophosphorus pesticides represented by dichlorvos, this biosensor has the potential to detect other AChE inhibitors, such as carbamate pesticides, drugs for Alzheimer's disease, etc., thus having broader applications in food safety and drug screening.
研究领域:
生物化学
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分析化学
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纳米技术
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环境科学
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DOI
PubMed
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 117
·96997-97002
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IF 3.84
Liwen Liang,Xu Fei,Yue Li,Jing Tian,Longquan Xu,Xiuying Wang,Yi Wang
We have synthesized a novel composite material with a hierarchical flower-like structure and extremely high enzyme activity. The spherical, hierarchical flower-like structure with numerous small flowers was formed through self-assembly using papain as the organic component and Cu3(PO4)2·3H2O as the inorganic component. This hybrid-nanoflower structure was confirmed by Fourier transform infrared spectroscopy, and X-ray diffraction. The enzyme activity of papain embedded in the hybrid nanoflowers was further evaluated using BAEE as a substrate. Compared with free papain in solution, the hybrid materials exhibited extremely high enzyme activity (∼4510%). A study on the relationship of enzyme weight percentage and pattern structure with enzyme activity revealed that enzyme activity was mainly affected by the material structure. These results demonstrate that this hierarchical structure can effectively increase enzyme activity.
研究领域:
材料科学
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生物化学
·
纳米技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Xinyu Li,Yuanye Pan,Jiayao Du,Hanchi Shi,Shuangqing Fan,Jinghan Li,Haijiao Xie,Minghui Cao,Siqi Li,Tong Liu
Structural evolution of Cu 3 (HHTP) 2 under polymerization is revealed. • Cu 3 (HHTP) 2 -derived species and PANI synergistically enhance NH 3 sensing. • The sensor achieves a wide NH 3 detection range of 0.5–500 ppm. • The sensor exhibits reliable sensing under high humidity and bending. • The sensor realizes real-time monitoring of seafood spoilage. Ammonia (NH 3 ) is a key volatile indicator of seafood spoilage, and developing sensitive NH 3 sensors that operate stably in complex environments is highly desirable. Conductive polymers such as polyaniline (PANI) have attracted attention for room-temperature sensing, but their limited adsorption capability and environmental stability still restrict practical applications. In this work, a flexible NH 3 sensor was developed by integrating PANI with Cu 3 (HHTP) 2 through in situ oxidative polymerization. During the acidic polymerization process, Cu 3 (HHTP) 2 undergoes structural evolution, generating Cu-containing and HHTP-derived components that remain associated with the PANI matrix. The optimized PACU20 sensor exhibits a wide detection range of 0.5–500 ppm NH 3 , a high response value of 14.5 toward 100 ppm NH 3 , and rapid response/recovery times of 37/56 s. Furthermore, the sensor maintains stable sensing performance under high humidity conditions and repeated bending cycles, indicating its robustness under practical storage and flexible operating environments. The enhanced sensing behavior might be attributed to the synergistic interaction between PANI and Cu 3 (HHTP) 2 -derived components, which regulate the local chemical environment of PANI and enhance NH 3 -induced charge variation. Practically, the sensor was applied to monitor ammonia evolution during fish and shrimp spoilage, demonstrating its potential for seafood freshness evaluation.
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DOI
高影响因子
Advanced Materials Interfaces
·
2021
·Vol. 8
·期 11
·2100308
·
IF 6.147
Weiwei Zhao,Tiantian Chen,Weikang Wang,Shuaihang Bi,Mengyue Jiang,Kenneth Yin Zhang,Shujuan Liu,Wei Huang,Qiang Zhao
2D conductive metal–organic frameworks (2D c-MOFs) naturally possess high active sites, large specific surface areas, and fast ion transport for energy-storage devices. However, the intelligent exploration of 2D c-MOFs for the emerging flexible transparent supercapacitors (FTSCs) with excellent photoelectric property and electrochemical activity is rarely implemented. Herein, 2D conductive ultrathin Cu 3 (HHTP) 2 (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene) film is synthesized on the indium tin oxide/polyethylene terephthalate (ITO/PET) substrate for flexible transparent conductive electrodes (FTCEs) through the layer-by-layer assembly method. The interconnected conductive frameworks possess the cooperative superiority of low internal resistance, fast electrolyte ion diffusion, and quick electron transfer. Cu 3 (HHTP) 2 -15/ITO/PET FTCEs show high photoelectric property of T 550 nm = 82.2% and R s = 49.1 Ω sq −1 , and high areal capacitance ( C A ) of 1700 µF cm −2 . The corresponding symmetrical FTSCs ( T 550 nm = 62.1%) exhibit excellent C A of 939.2 µF cm −2 at the current density of 7 µA cm −2 , superior rate capability (63.9% at 150 µA cm −2 ), long-term cycling stability (85% after 3000 cycles), and mechanical flexibility under different bending angles. This work provides key insights into the design and synthesis of 2D c-MOF films for flexible transparent energy-storage devices.
研究领域:
材料科学
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能源存储技术
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纳米技术
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DOI
高影响因子
Desalination and Water Treatment
·
2014
·
IF 0.987
Ling Li,Jun Cheng Li,Zhuang Rao,Gong Wu Song,Bin Hu
The adsorpion of methylene blue from aqueous solution on a highly porous metal-organic framework material [Cu3(BTC)2(H2O)3] was studied in conjunction with the adsorption isotherm, kinetics and regenerate of the sorbent. The adsorption isotherms of methylene blue on [Cu3(BTC)2(H2O)3] followed both the Freundlich isotherm and the Langmuir adsorption isotherm. Adsorption kinetics was determined from the experimental data, and the results showed that the adsorption obeyed a pseudo-second-order kinetics. The best oscillate time and the best [Cu3(BTC)2(H2O)3] amount were discussed, and [Cu3(BTC)2(H2O)3] gave high adsorption in only 5 minutes. The used [Cu3(BTC)2(H2O)3] could be regenerated by glycol solution, thus recycled. SEM image and FT-TR spectra of recycled [Cu3(BTC)2(H2O)3] after different adsorption times were compared. The high adsorption capacity and excellent reusability make [Cu3(BTC)2(H2O)3] attractive for the removal of methylene blue from aqueous solution.
研究领域:
环境科学
·
材料科学
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DOI
高影响因子
ANALYTICAL CHEMISTRY
·
2019
·
IF 6.35
Xiaofeng Tan,Xiaoying Wang,Lianhua Zhang,Luyao Liu,Gengxiu Zheng,He Li,Feimeng Zhou
Polydopamine (PDA)-coated or encapsulating Cu3(PO4)2 (Cu3(PO4)2@PDA) nanosheets were synthesized, allowing the C-reaction protein (CRP) antibody to be attached electrostatically for immunosensing of CRP with simple photothermal detection. The antibody-covered Cu3(PO4)2@PDA nanosheets replace the antibody-conjugated enzyme in the enzyme-linked immunosorbant assays. Owing to the high surface area of the 2-D-structured Cu3(PO4)2@PDA nanosheets and the coabsorption of light in the near-IR spectrum by Cu3(PO4)2 and PDA, a small amount of Cu3(PO4)2@PDA confined in the wells of a titer plate generates an easily detectable temperature change after irradiation at 808 nm. The temperature changes, measured by an inexpensive pen-type thermometer, increased linearly with the analyte concentration from 0.42 to 16 pM. We found that the linear relationship can be fitted by the isotherm derived from responses collected from heterogeneous sensors covered with different ligand or antibody densities. The low detection limit (0.11 pM) is largely due to the attachment of a great number of antibodies onto the flat nanosheets. The antibody-covered Cu3(PO4)2@PDA nanosheets are stable and can be used under conditions that are generally unfavorable to enzymatic activities. The excellent agreement between our results and immunoturbidimetric assays of CRP in serum samples from patients and healthy donors demonstrates its utility for disease diagnosis in clinical settings. This cost-effective, biocompatible, and convenient photothermal immunosensor affords a range of possibilities for detecting diverse protein biomarkers.
研究领域:
生物医学工程
·
分析化学
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DOI
PubMed
高影响因子
Advances in Materials Science and Engineering
·
2019
·
IF 1.399
Zhuo Yao,Dianli Qu,Yuxiang Guo,Yujing Yang,Hong Huang
Novel catalysts with high activity for the selective catalytic reduction of NO with NH3 (NH3-SCR) at low temperatures are highly demanded. In this study, mixed-node metal-organic frameworks (MOFs), e.g. Mn@CuBTC with controlled Mn composition in Cu3(BTC)2, were fabricated using postsynthetic exchange method and their structural characteristics and catalytic performances for NH3-SCR reaction were assessed. A series of analyses in terms of structure, surface morphology, texture, and chemical state determined that Mn ions were successfully incorporated into the Cu3(BTC)2 crystal lattice as well as adsorbed on the walls of nanopores in the framework. The pore sizes can be finely tuned in the presence of Mn ions in the cages, which significantly suppressed water adsorption. The NH3-SCR activity of Mn@CuBTC exhibited nearly 100% NOx conversion rate in the temperature range (230–260°C). The superior NH3-SCR performance is attributed to the proper pore sizes, reduced water content, and the synergistic effect between manganese and copper ions in the MOF structure, which enhanced NH3 bound to the active Lewis sites.
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
MATERIALS RESEARCH BULLETIN
·
2016
·
IF 2.435
Shuqiang Jiao,Jingjing Tuo,Hongliang Xie,Zihang Cai,Shuai Wang,Jun Zhu
Prussian blue analogues (PBAs) have recently attracted extensive interests as a new class of cathode materials for rechargeable batteries. Copper hexacyanoferrate, a typical Prussian blue analogue with the chemical formula Cu 3 [Fe(CN) 6 ] 2 , has been synthesized by solution precipitation method and investigated as a cathode material for sodium-ion batteries. The galvanostatic cycling tests show a specific capacity of 44 mA h g −1 at a current density of 20 mA g −1 , and the capacity retention can be 57.1% after 50 cycles. The material can also deliver a specific capacity of 37 mA h g −1 and 25 mA h g −1 at a rate of 50 mA g −1 and 100 mA g −1 , respectively. Furthermore, the material exhibits a high reduction peak at 3.32 V vs. Na + /Na, which brings more power to sodium-ion batteries. The data indicate the as-prepared material is capable of realizing the single electron redox capacity due to the reduction of Fe 3+ /Fe 2+ . All of the findings suggest a possible use of Cu 3 [Fe(CN) 6 ] 2 nanoparticles as environmental friendly and cost-effective cathode material, which also open new perspectives to develop cathode materials for sodium-ion batteries.
研究领域:
材料科学
·
电化学
·
能源存储
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DOI
高影响因子
FOOD CHEMISTRY
·
2019
·
IF 5.399
Nuan Feng,Haiyang Zhang,Yao Li,Yangkaixi Liu,Longquan Xu,Yi Wang,Xu Fei,Jing Tian
Milk allergenic proteins are the main reason of cow’s milk allergy. The most common method for removing milk allergenic proteins is enzymatic hydrolysis . However, the direct application of protease to hydrolyze allergens will lead to the introduction of new allergenic proteins. An ideal strategy for removing milk allergenic proteins without introducing new allergenic proteins is immobilization of protease. Herein, we established a simple method to synthesize a novel papain-Cu 3 (PO 4 ) 2 ·3H 2 O–magnetic nanoflowers (PCMNs). The PCMNs demonstrated 1556% higher activity than the free alkaline papain . Moreover, the PCMNs could hydrolyze most of allergenic proteins in cow’s milk, generating low-sensitive milk. In cycle analysis, the PCMNs also exhibited good reusability and were easily separated from the product.
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PubMed
高影响因子
ACS Applied Nano Materials
·
2023
·
IF 5.9
Junru Li,Yunqi Huang,Yanli Zhou,Hui Dong,Haoyuan Wang,Haoran Shan,Yifei Li,Maotian Xu,Xiaobing Wang
The conductive metal–organic framework (CMOF) is a promising application nanomaterial for the construction of electrochemical sensors. Three two-dimensional conductive M3(HHTP)2 materials with larger aspect ratios were prepared by a one-pot method using acetate-based metals (Cu, Ni, Co) and 2,3,6,7,10,11-hexahydroxytriphenylene (HHTP) with the introduction of N,N-dimethylformamide (DMF) as the limiting reagent. Compared with Ni3(HHTP)2 and Co3(HHTP)2, Cu3(HHTP)2 had a larger double capacitance, pore size, specific surface area, and smaller resistance. As a result, Cu3(HHTP)2 provided greater catalytic oxidation active surface area and charge transfer efficiency for malachite green (MG) detection. Hence, Cu3(HHTP)2 efficiently catalyzed MG oxidation and significantly improved the sensitivity of MG detection. Meanwhile, the oxidation current signal from the copper of Cu3(HHTP)2 was used as an internal reference signal to form a ratiometric electrochemical sensor with an MG oxidation current signal, which effectively reduced the external interference. The constructed electrochemical assay for MG detection displayed broad linearity (5–1000 nM) with a detection limit of 1.34 nM. In the meantime, MG residues in fish was evaluated and high reliability was obtained, confirming the feasibility of this valuable method for food safety and health evaluation of aquatic products.
研究领域:
材料科学
·
分析化学
·
食品安全
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）