JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Yonglong Huang,Zhengkang Duan,Chuan Li,Tian Qiu
The catalytic dehydrogenation of diethanolamine to prepare iminodiacetic acid has attracted considerable research interest. However, the lack of understanding of the structure-activity relationship of the reaction can present a challenge to the control of the catalytic behavior. Concurrently, improving the catalytic performance and reducing the cost have also become urgent issues that require resolution. This work examined the catalytic mechanism of several Cu-Ni X /ZrO 2 catalysts, differing in Cu/Ni ratios, prepared by H 2 reduction, in the context of DEA dehydrogenation to elucidate the structure-activity connection and probable reaction mechanism. Subsequently, a strategy has been put out to generate metal (Ni and Co)-doped copper-zirconium catalysts using the co-precipitation-hydrazine hydrate reduction process. The synergistic effect between metals was combined with the improvement of the surface reaction of the catalyst by hydrazine hydrate through a more efficient preparation method, thereby enhancing the catalyst's overall performance. The representative catalyst Cu-Ni/ZrO 2 required a hydrazine hydrate reduction temperature and time of 40 °C and 30 min, and after 65 min of reaction, it exhibited a high conversion rate (96.3 %) and yield (93.7 %), and after five cycles, both the conversion rate and yield exceeded 85 %. Various characterization techniques have confirmed that Ni doping induced an alloying effect and a size effect. Additionally, the hydrazine hydrate reduction method was discovered to augment the specific surface area, surface hydroxyl groups, hydrophilicity, and optimize the pore size distribution of the catalyst while also regularizing its morphology, thereby significantly enhancing the activity and stability of the metal-doped copper-zirconium catalyst. This paper discussed the correlation between catalyst structure and reaction performance, as well as the catalytic conversion mechanism, which is anticipated to provide a novel reference for the preparation, performance control, and potential applications of dehydrogenation catalysts.
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INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
·
IF 7.7
Aowei Lv,Xue Lv
Anthropogenic wastewater generation and water pollution can have negative impacts on public health and ecosystems. However, most materials do not have both adsorptive and catalytic properties, so the design and development of sustainable and multifunctional materials is essential for wastewater treatment. Herein, composite hydrogel (PHG) containing [2-(Methacryloyloxy)ethyl]dimethyl-(3-sulfopropyl) ammonium hydroxide (SBMA) and chitosan quaternary ammonium salts (HACC) were prepared for wastewater treatment. The adsorption capacities of the PHG hydrogels for nickel (Ni II ), copper (Cu II ), and palladium (Pd II ) ions were 158.68, 182.99, and 229.78 mg/g, respectively. The adsorption process is consistent with the Langmuir adsorption model and quasi-secondary kinetics. For further application of adsorbed metal ions, NaBH 4 was selected for in situ reduction to prepare hydrogel-based catalysts cemented with metal nanoparticles (Ni-, Cu- and Pd-NPs), respectively. The PHG-Pd catalysts demonstrated significant catalytic efficiency in reducing 4-nitrophenol and methylene blue, and K app were 0.307 and 0.365 min −1 , respectively. Among them, the activation parameters for the reduction of 4-NP over PHG-Pd catalyst were calculated as E a = 36.27 kJ/mol, ΔH # = 33.72 kJ/mol and ΔS # = −259.68 J/(mol·K). This study is expected to provide insights into the design of multifunctional adsorption catalysts for the removal of dyes and nitro compounds from wastewater.
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ACS Applied Energy Materials
·
2024
·
IF 5.4
Hao Shi,Haozhen Li,Xing Zhou,Chongqing Yang,Hengyong Tu,Jun Tong,Longkai Xiang,Chao Ma,Lei Zhu,Zhen Huang
Spinels have been widely employed as contact layers (CLs) on metallic interconnects for solid oxide cells (SOCs) with the required electrical conductivity and Cr block ability. In this work, MnCo2O4 spinels doped with different transition metals (Cu, Ni, and Zn) were deposited on precoated SUS441 stainless steel as CLs. A positive doping effect of Cu and Ni on increasing the concentration of Mn4+/Mn3+ and Co3+/Co2+ hopping pairs was observed, whereas a negative doping effect of Zn on electrical conductivity was confirmed, which was reflected in the data of X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectra (XAS). The Cu-doped Mn1Co1.7Cu0.3O4 spinel exhibited the best electrical conductivity with a low area specific resistance (ASR) value of 4.5 mΩ·cm2 at 850 °C. A relative degradation test demonstrated that Mn1Co1.7Cu0.3O4 maintained significant performance during a 200 h isothermal process. Cross-sectional observations revealed that the thickness of the Cr oxide scale formed during the degradation test was much reduced by the Mn1Co1.7Cu0.3O4 CL, which was attributed to the improved resistance to Cr oxidation. The present work shed light on the design of highly conductive CLs in SOCs.
研究领域:
材料科学
·
能源科学
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CERAMICS INTERNATIONAL
·
2026
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IF 6
Chengkai Li,Changjian Zhou,Ze Liu,Zhenyu Zhang,Danni Zeng,Rongfeng Guan
Driven by the dual demands of global energy structure transformation and carbon neutrality goals, solar-driven green hydrogen and green chemical synthesis have become a focus. This study employs a Prussian blue template to guide the one-step synthesis of Cu/Ni co-doped Cd 0.9 Zn 0.1 S, which not only retains a high-surface-area porous framework with exposed active sites but also intentionally introduces abundant sulfur vacancies (Vs). The synergistic interplay of Cu doping (acting as electron-rich centers), Ni doping (serving as hole-trapping centers), and the generated V s collectively optimizes the band structure, extends light absorption to nearly 700 nm, and significantly enhances charge carrier separation. The optimized 10Cu/10Ni- Cd 0.9 Zn 0.1 S photocatalyst achieves an exceptional hydrogen production rate of 21.25 mmol g −1 h −1 (20-fold enhancement) and a H 2 O 2 production rate of 4.6 mmol g −1 h −1 under oxygen conditions (15-fold enhancement). Remarkably, the in-situ generated H 2 O 2 is efficiently activated on Cu/Ni sites and Vs via a photo-Fenton-like process, enabling rapid tetracycline degradation (94% within 40 min). DFT calculations reveal that the hydrogen adsorption free energy is optimized to −0.09 eV, and the introduced sulfur vacancies further lower the work function, promoting O 2 activation and charge transfer for both H 2 evolution and Fenton-like reactions. This study offers new insights into designing highly efficient photocatalysts by employing a coupled doping and vacancy engineering strategy to synergistically regulate redox-active sites, combining porous framework design for optimized mass transport and multifunctional environmental remediation.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 23
·10020-10032
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IF 9.8
Qiyuan Zheng,Li Zeng,Zuoying Cao,Shengxi Wu,Qinggang Li,Mingyu Wang,Wenjuan Guan,Guiqing Zhang
As the production of electric vehicles and lithium-ion batteries continues to rise, concerns over resource scarcity and supply shortages of critical metals, including Cu, Ni, Co, Mn, and Li, have become increasingly urgent. To address these concerns and promote environmental protection, there is a growing demand for the recycling of hazardous waste containing these critical metals as secondary resources. Therefore, this paper proposes a novel synergistic solvent extraction system of D2EHPA-NNPA, which fills a gap in the lack of a suitable extraction system for the hydrometallurgical industry of secondary resources containing Cu, Ni, Co, Mn, and Li. With the specific extraction sequence of D2EHPA-NNPA, a novel process has been designed and proposed for the stepwise extraction of Cu, Ni, Co, Mn, and Li from secondary resources, which significantly simplifies process flows while avoiding cross-contamination of the extractants and the production of industrial wastewater. Furthermore, the proposed “extraction-scrubbing-stripping” process has been investigated from both macroscopic and microscopic perspectives, demonstrating that the novel synergistic solvent extraction system of D2EHPA-NNPA is a viable option for industrial applications to promote a circular economy and achieve sustainability objectives.
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Catalysts
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2024
·Vol. 14
·期 8
·496
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IF 3.8
Kaige Zhao,Xinhao Xu,Manli Wang,Tao Chen,Qianlin Ju,Lulu Hao,Zelin Chen,Xiaolong Yu,Changjiu Li
The electrocatalytic oxidation of urea combined with wastewater splitting is considered a promising approach for sustainable hydrogen production, characterized by minimal energy consumption. However, its evolution is greatly hindered by the shortage of efficient and easily accessible electrocatalytic materials. Here, a facile electrochemical activation strategy was conceived and proposed to construct a Cu-doped NiOOH nanolayer encapsulated on Cu2O nanodendrites on Cu mesh substrate (Cu-NiOOH/Cu2O/CM) from the electrodeposited Ni/Cu2O/CM heterostructured precatalyst. It was verified that the incorporation of Cu not only facilitates the rapid formation of Ni(III)species but also contributes to the formation of Cu-Ni(III)bifunctional electrocatalytic active sites. Benefiting from the accessible Cu-Ni(III)dual active sites, high active surface area, good hydrophilic and aerophobic surface properties and superior electrical conductivity of the Cu mesh substrate, the as-prepared Cu-NiOOH/Cu2O/CM exhibits enhanced bifunctional electrocatalytic abilities for electrocatalytic urea oxidation reaction (UOR) and hydrogen evolution reaction (HER). Particularly, for the Cu-NiOOH/Cu2O/CM||Cu-NiOOH/Cu2O/CM configuration toward the UOR||HER coupled system, a significantly reduced cell voltage of 1.43 V vs. RHE @ 10 mA·cm−2was obtained. The observed cell voltage for the conventional overall water splitting is approximately 190 mV higher than that observed for overall urea splitting. This study proposes a viable approach to achieve and optimize the bifunctional UOR/HER performance of NiOOH active species, which holds significant importance for efficient and stable hydrogen generation from urea-contaminated substandard water.
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BIOSENSORS & BIOELECTRONICS
·
2017
·
IF 7.78
Yaoguang Wang,Guanhui Zhao,Xiaojian Li,Li Liu,Wei Cao,Qin Wei
In this work, a highly-efficient competitive method-based electrochemiluminescence (ECL) immunosensor was proposed based on {[Ru(bpy) 3 ][Cu 2x Ni 2(1−x) (ox) 3 ]} n (Cu/Ni/Ru) as luminophor to efficiently detect aflatoxins B1 (AFB1). Cu/Ni/Ru exhibited excellent ECL behavior. While polyethyleneimine capped silicon dioxide (PEI@SiO 2 ) could decrease the ECL performance of Cu/Ni/Ru due that PEI could destroy the structure of Cu/Ni/Ru via producing the complex between PEI and metal ions (Cu(II)/Ni(II)), inducing the release of Ru(bpy) 3 2+ . Since Au nanoparticles can directly combine with antibody and antigen, the Cu/Ni/Ru and PEI@SiO 2 was functionalized by Au nanoparticles . The quantitative detection of AFB1 was based on the competitive binding between AFB1-bovine serum albumin labeled Au-PEI@SiO 2 (Au-PEI@SiO 2 -AFB1-BSA) and free AFB1 with antibody-AFB1 which immobilized on Au-Cu/Ni/Ru. The ECL signal increased with augmenting the concentrations of the free AFB1 due to less Au-PEI@SiO 2 -AFB1-BSA combining with antibodies. Under optimal conditions, the proposed immunosensor exhibited a wide linear range from 0.01 ng mL −1 to 100 ng mL −1 with a detection limit of 0.0039 ng mL −1 (S/N = 3). The proposed immunosensor also provides a promising approach for ultrasensitive detection of other mycotoxins .
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Qiyuan Zheng,Shengxi Wu,Qinggang Li,Mingyu Wang,Wenjuan Guan,Zuoying Cao,Guiqing Zhang
Developing a novel extraction process for battery minerals-nickel laterites is a key aspect of building a resilient and low-carbon future, as the current process produces heavy metal residues, electrolytic wastewater, and toxic gases, while also facing issues of long process flow and low resource utilization. The primary bottlenecks in the process stem from the low separation coefficients and poor selectivity of commercial extractants. In this paper, a novel synergistic solvent extraction (SSX) system, dinonylnaphthalenesulfonic acid (DNNSA)-N,N-bis(pyridin-2-ylmethyl)tetradecan-1-amine (NNPA), has been proposed to address the bottlenecks. Based on the DNNSA-NNPA SSX system, a novel hydrometallurgical process has been proposed for the stepwise extraction of valuable metals from nickel laterites. In the proposed process, Cu, Ni, Co, and Zn were directly extracted from the nickel laterite leachate, reducing their concentrations to below 1 mg/L. The enriched metals were subsequently separated as CuSO4, NiSO4, CoSO4, and ZnSO4 solutions, each with a purity exceeding 99.9%. Thereafter, Cr, Fe(III), and Al were sequentially removed from the raffinate through stepwise precipitation, achieving their preliminary separation. Mn was then selectively extracted from the resulting precipitate–mother liquor, yielding a high-purity MnSO4 solution (>99.9%). This integrated approach enables the comprehensive resource extraction of nickel laterites. Systematic mechanistic studies and pilot plant tests demonstrate that the novel extraction process significantly improves metal ion separation coefficients, avoids coprecipitation losses of Ni and Co, simplifies the process flow, avoids hazardous waste generation, reduces energy consumption, and improves resource utilization.
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