JOURNAL OF PHOTOCHEMISTRY AND PHOTOBIOLOGY A-CHEMISTRY
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2024
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IF 4.1
Meng-Jie Cui,Shan-Shan Li,Tie-Zhen Ren,Abulikemu Abulizi,Ai-Sha Nulahong
H 2 evolution through photocatalysis possesses has the advantage for achieving the carbon neutral, that relies on the highly efficient catalysts. Non-noble metals have lower prices than noble metals, which is beneficial for their large-scale applications in industry. In this paper, functionalized CuNi alloy and BaTi 4 O 9 (BTO) composite (Cu x Ni y /BTO(Z)) photocatalyst were synthesized successfully through hydrothermal calcination method. The acetates were selected the raw material to avoid the use of hazardous chemicals and pollution of photocatalysts by other elements, while also providing C=O for the photocatalyst to further enhance its photocatalytic activity. Under visible light irradiation, the photocatalytic hydrogen (H 2 ) evolution rate of Cu 3 Ni/BTO is 184.14 μmol·g −1 ·h −1 , which is 101.18 times that of pure BTO (1.82 μmol·g −1 ·h −1 ) under the same conditions. Combining density functional theory (DFT) calculations and experimental studies, it is concluded that electronic structural characteristics of BaTi 4 O 9 and the addition of CuNi alloy could provide more electrons and improve the photocatalytic H 2 evolution activity.
研究领域:
材料科学
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能源科学
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化学工程
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DOI
高影响因子
Surfaces and Interfaces
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2024
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IF 5.7
Zhiwei Zou,Hongxiang Zhang,Xuefeng Pan,Hui Shen,Jianying Yu,Tengfei Guo,Yonghao Wang
Electrocatalytic reduction of nitrate (NO 3 - ) to ammonium (NH 4 + ) is an environment friendly approach for treating nitrogen-containing wastewater. Consequently, electrocatalysts capable of effectively and selectively reducing NO 3 - to NH 4 + receives growing attention. However, Cu-based catalysts demonstrate limited efficiency and the drawback of generating toxic NO 2 - though it is prevalent in the field of electrocatalytic reduction of NO 3 - (NO 3 RR). In this work, a CuNi alloy was synthesized on a Co foil through electrodeposition (marked as CuNi@Co) and its electrocatalytic performance for NO 3 RR was evaluated. XRD, EDS mapping and XPS characterization indicate CuNi exists with alloy state. Electrocatalytic experiments demonstrate that CuNi@Co exhibits an exceptional FE NH3 of 99.12% at -0.64 V (vs. RHE). Importantly, no detrimental NO 2 - generated during NO 3 RR process because the reduction rate from NO 2 - to NH 4 + is faster than that from NO 3 - to NO 2 - . Mechanistic analysis suggests that Cu serves as a ‘reservoir’ to provide electrons to facilitate the reduction of NO 3 - to NO 2 - during NO 3 RR process and the synergistic effect of Ni and Cu promotes more active hydrogen (H*) to participate the reduction process of NO 2 - to NH 4 + not H 2 generation, ultimately improving FE NH3 . This work elucidates the role of electrons and H* in electrocatalytic nitrate reduction to ammonium for CuNi alloy, providing new insights into the reduction process of NO 3 RR for Cu-based materials.
研究领域:
环境科学
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电催化
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材料科学
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DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2024
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IF 5.8
Xiang Ji,Yaodong Yu,Aixin Ma,Yujia Guan,Hongdong Li,Jianping Lai,Lei Wang
Nitrate (NO 3 - ) and hydrazine (N 2 H 4 ) are common nitrogen pollutants in groundwater. The electrochemical method can be used to synthesize the added product urea while treating N-pollution. Therefore, the development of sufficiently efficient electrosynthesis urea systems and efficient electrocatalysts is of great significance, but also challenging. In this paper, CuNi alloy nanosheets (Cu x Ni y /CF) on copper foam surface were synthesized by electrodeposition, and C-N coupled hydrazine oxidation (HzOR) system was constructed by proton exchange membrane (PEM). Cu and Ni in CuNi alloy act as double active sites and react with C-N coupling reaction and HzOR respectively. At −0.5 V potential, the Faraday efficiency of Cu 8 Ni 2 /CF for C-N coupling reaction is 51.66 %, and the urea yield is 254.09 μg h −1 cm −2 . At the same time, HzOR with low thermodynamic oxidation potential can quickly produce excess H + to supply protons to the cathode for C-N coupling reaction, thus significantly promoting the forward C-N coupling reaction. Cu 1 Ni 9 /CF also showed significant activity in the oxidation reaction of N 2 H 4 in KOH electrolyte. Therefore, we assembled a Cu 1 Ni 9 (+) || Cu 8 Ni 2 (-) electrolytic cell, which only needs 0.23 V working voltage up to 150 mA cm −2 , and can convert NO 3 - and CO 2 to urea at a power consumption of 5.09 kWh kg −1 while converting N 2 H 4 . Energy saving 37.6 % compared to conventional C-N coupled OER electrolytic system (about 8.16 kWh kg −1 urea). It can greatly reduce the cost of urea production, make the price of fertilizer and chemical raw materials more competitive, and promote the development of agriculture and chemical industry while reducing greenhouse gas emissions and nitrogen pollutants in the ecological environment. This study reports a promising and effective strategy for the synthesis of urea and treatment of N contaminants at a small operating voltage.
研究领域:
环境科学
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材料科学
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化学工程
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产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
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2022
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IF 4.05
Yu Nanxi,Lu Houfang,Yang Wei,Zheng Yuxin,Hu Qiang,Liu Yingying,Wu Kejing,Liang Bin
In the process of converting biomass into high value-added chemicals, transfer hydrogenation as a mild hydrogenation method has attracted more and more attention. The catalysts with hydrogenation sites (nano CuNi alloy) and acid sites (Al oxide) highly dispersed on the surface of a stable support (active carbon) were prepared and the importance of acid sites for the activity of CuNi catalysts in transfer hydrogenation was demonstrated. The catalysts showed promising catalytic activity on the transfer hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL). The CuNi-1Al/AC with 5 wt.% CuNi alloy and 5 wt.% Al got 97.2% GVL yield and 100% LA conversion at 220 ℃ in isopropanol for 2 h. The high activity of the catalyst is attributed to the promoted esterification by the supported acid sites. The Al-modified catalyst also showed activity for esterification reaction in different alcohol hydrogen donors. The catalyst occurs inactive during the cycle due to the shedding of the active components, and the stability of catalyst is effectively improved by a stepwise impregnation. Graphical abstract
研究领域:
催化化学
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可再生资源化学
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DOI
高影响因子
DALTON TRANSACTIONS
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2020
·Vol. 49
·期 16
·5074-5086
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IF 4.174
Hua Jiang,Shuaiqi Gong,Shu Xu,Penghui Shi,Jinchen Fan,Volkan Cecen,QunJie Xu,YuLin Min
A major challenge in the field of photocatalytic carbon dioxide (CO2) reduction is to design catalyst systems featuring high selectivity for CO production, long-term stability and a composition of Earth-abundant elements. Here, we present a metal–organic framework (MOF) based catalyst to mitigate the technical problems associated with the above-mentioned features. We report a carbon-coated CuNi alloy nanocatalyst obtained by high temperature vacuum treatment of a MOF material (CuNiBTC). The resulting carbon encapsulated CuNi (denoted as CuNi/C) nanoparticles possess a well-designed core–shell composite structure with graphene shells. Meanwhile, we investigated the reaction mechanism of CO2 on the surface of the CuNi/C photocatalyst in an aqueous solution containing triethanolamine. The experimental results show that the activity and catalytic yield of CuNi/C are much higher than those of Cu/C and Ni/C alone. At the same time, the catalytic activity of CuNi/C is also affected by changing the reaction temperature in the preparation process. As a result, the CuNi/C samples can achieve nearly 90% selectivity for NIR-light-driven CO2 reduction to CO. Our approach demonstrates the potential of non-semiconductor materials as catalysts for efficient and selective reduction of CO2 to CO.
研究领域:
材料科学
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环境科学
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产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2021
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IF 3.764
Hongbin Shi,Xiaofeng Dai,Qing Liu,Teng Zhang,Yabing Zhang,Yuling Shi,Tao Wang
Magnetic CuNi alloy nanoparticles (CuNi NPs) for the catalytic transfer hydrogenation (CTH) of nitroarene were successfully prepared by the facile thermal decomposition of copper formate (Cuf) and nickel formate (Nif) simultaneously. Liquid paraffin served as solvent, and oleylamine (OAM) acted as both complexing agent and stabilizer. The particle size and Cu/Ni composition of CuNi NPs could be controlled by adjusting the amount of OAM and the Cu/Ni ratio of the precursor. The average diameter of the prepared CuNi NPs ranged from 10.2 to 56.9 nm. It had been confirmed that CuNi NPs were an alloy of Cu and Ni and effectively resistant to oxidation. The prepared CuNi NPs could be separated under an external magnetic field without any energy consumption since they were superparamagnetic. Among the prepared CuNi NPs with different compositions, the Cu3Ni7 NPs were the best catalyst for catalytic transfer hydrogenation of nitrobenzene with ethylene glycol (EG) as the hydrogen donor, giving a nitrobenzene conversion of 99% and an aniline yield of >97%. The conversion and yield remained above 95% and 80% respectively after 10 cycles of NOBF4-treated Cu3Ni7 NPs, demonstrating good reusability for the CTH reaction. This work reported a novel method for preparing magnetic CuNi NPs and also provided a new approach for the hydrogenation of nitroarene catalyzed by non-noble metals in a green environment.
研究领域:
材料科学
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催化化学
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环境科学
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产品关联
DOI
高影响因子
JOURNAL OF MATERIALS SCIENCE & TECHNOLOGY
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2025
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IF 14.3
Beibei Gao,Yi Zhou,Yuan Fang,Richeng Jin,Yuchi Fan,Lianjun Wang,Wan Jiang,Pengpeng Qiu,Wei Luo
Mesoporous framework supported metal nanoparticle catalyst represents a promising material platform for creating multiple active sites that drive tandem reactions. In this study, we demonstrate a novel catalyst design that involves the encapsulation of CuNi alloy nanoparticles within mesoporous silicon carbide nanofibers (mSiC f ) to achieve efficient tandem conversion of furfural (FFA) into 2-(isopropoxymethyl)furan (IPF). The unique one-dimensional (1D) mesoporous structure of mSiC f , coupled with abundant oxygen-containing groups, offers a favorable surface microenvironment for the stabilization of bimetallic CuNi active sites. Through carefully optimizing metal to acid sites, we have developed a catalyst containing a total mass ratio of 20 % Cu and Ni, which exhibits a remarkable performance with complete FFA conversion and 92 % IPF selectivity in 4 h. In-depth mechanistic investigations have revealed that the superior activity of this catalyst is attributed to a tandem reaction mechanism. Initially, FFA is hydrogenated at the dual metal active sites to produce furfuryl alcohol (FOL) as an intermediate, which is subsequently etherified at the acid sites with suitable species and strengths on the mSiC f supports. Additionally, the robust 1D mSiC f framework effectively protects the metal sites from agglomeration, resulting in excellent reusability of the catalyst. This study underscores the potential of mesoporous silicon carbide-supported bimetallic active sites for achieving enhanced tandem catalytic functionality.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2024
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IF 7.1
Ying Wu,Wenhui Fang,Min Li,Yutao Cao,Wei Cui,Zengxi Li,Hong Zhao
Electrochemical upgrading of biomass waste (such as glycerol)-assisted water electrolysis for the production of valuable formate and high-purity hydrogen offers a promising route to develop sustainable and clean sources of energy. Herein, using a simple two-step electrodeposition method to implant CuNi alloy in VOx-doped Ni (NiVOx), we construct a competent, stable, and bifunctional heterogeneous catalyst (CuNi–NiVOx) toward hydrogen evolution reaction (HER) and glycerol electrooxidation reaction (GER). The CuNi–NiVOx electrode presents excellent HER activity with an ultralow overpotential of 8 mV in 1.0 M KOH to deliver a current density of 10 mA cm–2 and high GER activity for selective formate production with high Faradaic efficiency (FE). Moreover, the hybrid electrolytic cell formed by the bifunctional CuNi–NiVOx catalyst was able to reach a current density of 10 mA cm–2 with an ultralow voltage (1.308 V). X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) calculations confirm the existence of electron transfer between the O sites and metal sites and between heterogeneous interfaces, thus optimizing the hydrogen adsorption ability (0.02 eV). This work may provide ideas for the engineering of heterogeneous dual-function electrocatalysts for energy-saving hydrogen production and simultaneous highly selective production of formate.
研究领域:
电化学
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催化
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能源材料
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可再生能源
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）