Carbon Energy
·
2025
·
IF 24.2
Mengmeng Ma,Runkang Lin,Kaige Huang,Shizhong Yue,Maohong Fan,Zhijie Wang,Shengchun Qu
Functionalization has emerged as a pivotal endeavor to tailor the surface properties of photocatalysts. We propose a facile amine functionalization strategy to establish a Cu−In−Zn−S (CIZS)/NiS x hybrid with covalent bonds using individual ethylenediamine (EDA) molecules. Our approach witnesses a remarkable photocatalytic hydrogen evolution (PHE) competence of 65.93 mmol g −1 h −1 driven by visible light, the highest value yielded by CIZS to date. X-ray absorption spectra of CIZS and density functional theory (DFT) calculations confirm the crucial amine N→Cu coordination after amine functionalization. The new emerging coordination via lone-pair electron donation profitably accesses the regulation of the coordination environment, electronic structures, and carrier behavior. Moreover, individual EDA molecule with two-terminal −NH 2 group serves as a molecular bridge to hybrid CIZS and NiS x cocatalyst via N→Cu and N→Ni coordination, favorably promoting efficient charge transport. This study provides advances in practical functionalizing photocatalysts.
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高影响因子
ACS Applied Materials & Interfaces
·
2025
·
IF 8.2
Minghan Wu,Siqi Hao,Linfeng Qi,Yu Shi,Wei Yang,Jingjing Bao,Min Du,Zhengyu Mo,Licheng Sun
Thermogalvanic cells (TGCs) are at the forefront of effective thermoelectric conversion methods, but the practical utilization of their integrated devices is hindered by the suboptimal performance of N-type TGCs. Herein, a novel redox couple of Cu/Cu(en)22+ is proposed to construct a liquid-state N-type TGC. The electrochemical reaction involving the Cu electrode, ethylenediamine (en), and their chelated compound Cu(en)22+ exhibits a significant reaction entropy change, resulting in an enhanced temperature coefficient (α). We reveal that the α of the Cu/Cu(en)22+-based TGC reaches 1.64 mV K–1. Furthermore, by optimizing the concentrations of Cu2+, ethylenediamine, and (NH4)2SO4 in the electrolyte, both α and normalized power density can be significantly improved, achieving values of 2.12 mV K–1 and 676 μW m–2 K–2, respectively. Moreover, by constructing a P–N junction with P-type and N-type TGC, we achieve a high potential of 121 mV under a temperature gradient of 35 K. This work expands the available redox couple options for N-type TGCs and offers a new pathway for efficient thermoelectric conversion.
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PubMed
高影响因子
CATALYSIS LETTERS
·
2017
·Vol. 148
·期 1
·181-193
·
IF 2.799
Lin Jin,Guo Yafei,Chen Xiao,Li Changhai,Lu Shouxiang,Liew Kim Meow
Abstract Nanostructured CeO 2 supported CuO–MnO 2 (CuMn/Ce) catalysts were synthesized by wet co-impregnation method and compared with CuO/CeO 2 and MnO 2 /CeO 2 catalysts on CO oxidation. The former shows significantly higher catalytic activity toward CO oxidation than the bimetallic oxides catalysts with minimum T 50 . Dual synergistic effects in the interfaces of CuO–MnO 2 and CuO–CeO 2 shall be responsible for the higher oxidation performance of CuMn/Ce catalyst. As Cu/Mn mass ratio varies from 1/0.2 to 1/9, CO oxidation activities of the catalysts present unimodal distribution, and the catalyst with Cu/Mn = 1/1 shows the highest performance (T 50 = 45.8 °C; Ea = 24.11 kJ mol −1 ). Cu acts as CO dissociative adsorption sites, and Mn–Ce supplies activated O species from gas molecule and lattice oxygen, which are both indispensable for improving utilization efficiency of the reactants in the dual redox processes. The catalytic performance of catalyst is also vitally correlated with calcination temperature (160–320 °C). The optimum calcination temperature of CuMn/Ce catalyst is 320 °C. Catalyst characterization results indicate that the pretreatment at 320 °C is decent to obtain desired metal oxides along with fine texture properties. Graphical Abstract
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高影响因子
Green Energy & Environment
·
2022
·
IF 12.781
Bolin Wang,Chunxiao Jin,Shujuan Shao,Yuxue Yue,Yuteng Zhang,Saisai Wang,Renqin Chang,Haifeng Zhang,Jia Zhao,Xiaonian Li
Rational design of catalytic sites to activate the C C bond is of paramount importance to advance acetylene hydrochlorination. Herein, Cu sites with electron-rich and electron-deficient states were constructed by controlling the impregnation solutions. The π electrons flowing from acetylene to Cu site are facilitated over the electron-deficient Cu sites, achieving high activation of C C bond. The contradiction between the increased activation of acetylene required for enhanced catalytic activity and the resistance of Cu site to reduction by acetylene required for maintaining catalytic stability can be balanced by establishing strong interactions of Cu site with pyrrolic-N species. The catalytic activity displays a volcano shape scaling relationship as a function of Cu particle size. Tribasic copper chloride is concomitantly generated with the construction of electron-deficient Cu sites. The H–Cl bond of HCl can be activated over the tribasic copper chloride, accelerating the surface reaction of vinyl chloride production. This strategy of inducing electron deficiency provides new insight into the rational design of catalysts for the synthesis of vinyl chloride with a high catalytic performance.
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高影响因子
Journal of Materials Chemistry C
·
2018
·Vol. 6
·期 30
·8105-8114
·
IF 5.976
Ping Gao,Xiang-Ying Sun,Bin Liu,Hui-Ting Lian,Xin-Qiang Liu,Jiang-Shan Shen
Developing a catalyst with a uniform and well-defined crystal structure is very important to establish a catalytic sensing system with high efficiency. In this work, Cu-BTC metal–organic frameworks (MOFs) without a crystalline CuO or Cu2O phase were successfully synthesized by using a low temperature synthesis method, and the as-prepared Cu-BTC MOFs were found to have outstanding catalytic activity towards the traditional oxidase substrate, o-phenylenediamine (OPD), to generate a colored and fluorescent product. The results of the kinetics analysis revealed that the catalytic behavior of Cu-BTC MOFs towards OPD could well follow the typical Michaelis–Menten equation, indicative of a strong affinity between Cu-BTC MOFs and OPD. On the basis of these findings, taken together the condensation reaction between the –CHO group of formaldehyde and the –NH2 group of OPD to form Schiff base compounds, a novel Cu-BTC MOF-based catalytic sensing system for detecting gaseous formaldehyde could be successfully established.
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高影响因子
MATERIALS CHEMISTRY AND PHYSICS
·
2017
·
IF 2.084
Dongfang Wu,Qingqing Tan,Lichong Hu
A highly selective morphology formation of Cu-Ni bimetallic nanocrystals is developed with a solvothermal method, using poly(vinylpyrrolidone) (PVP) as capping agent and aniline as reducing agent in benzyl alcohol. It is shown that temperature is crucial to the controlled synthesis of nanocrystals, and that Cu-Ni nanoparticles evolve from hexagonal nanoplates to nanowires with increasing the concentration of pyrrolidone unit. The synthetic Cu-Ni hexagonal nanoplates and nanowires are well dispersed and have high crystallinity , purity, uniformity of shape and size, and face-centered cubic lattice structure. Furthermore, a mechanism of the formation of Cu-Ni nanocrystals is proposed, and the functions of capping agent, reducing agent, solvent, etc. are discussed. It is also found that both nanoplates and nanowires show better catalytic activities in o -xylene combustion than the conventional catalyst. Especially, the Cu-Ni nanowire catalyst exhibits the most excellent catalytic performance due to the formation of durian-like surface structure.
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2018
·
IF 3.141
Xiaofeng Dai,Wen Xu,Teng Zhang,Tao Wang
Copper nanoparticles (Cu NPs) are a potential material for conductive inks because of their low price, high conductivity, and high electromigration resistance. However, Cu NPs are prone to be oxidized in air, which is lethal to conductivity. In this work, we report on the self-reduction of Cu NPs which are synthesized by the thermal decomposition of copper formate (Cuf) using oleylamine (OAM) as the complexing ligand and stabilizing agent. Although the particle surface partially oxidized to Cu2O in air, the cuprous oxide could be reduced to copper during sintering, because of the release of H2 through the decomposition of OAM adsorbed on Cu NPs. This self-reduction ability without the help of additional reduction agent makes the Cu NPs a promising material for conductive inks. The feasibility to formulate conductive ink with the prepared Cu NPs is demonstrated.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Hui Xu,Yuhang Zhong,Dingke Wang,Ran Sun,Yujie Tan,Xingang Liu,Jianyuan Hou,Yuan Yuan,Ximan Dong,Renxi Zhang
Cu/Z-700 enables plasma-driven H₂ evolution from simulated seawater vapor. • Dynamic Cu redox cycling acts as an electron relay during plasma catalysis. • Cu clusters, Cu N sites, and pyridinic N perform differentiated functions. • An H₂ rate of 1.33 mL min −1 is achieved with >95% activity after five cycles. How different active sites cooperate under non-thermal plasma (NTP) conditions is still poorly understood. Here, Cu-doped ZIF-8-derived carbon carbonized at 700 °C (Cu/Z-700) is shown to host three distinct active centers: metallic Cu clusters, Cu–N coordinated (Cu–NC) moieties and pyridinic N (Py-N) sites. Cu K-edge X-ray absorption spectroscopy reveals that ~80% of Cu exists as metallic clusters and ~ 20% as isolated Cu δ+ –Nₓ sites. Density functional theory (DFT) calculations suggest a functional division among the three sites: Cu clusters show the strongest Cu–OH binding and the most favorable reaction free energies, Cu–NC sites favor intermediate conversion and product desorption, and Py-N sites promote water adsorption. In a dielectric barrier discharge (DBD), Cu/Z-700 delivers a H₂ production rate of 1.33 mL min −1 from water vapor generated from simulated seawater at a residence time of 3 s, an 11-fold enhancement over plasma alone, with 93.6% activity retention over 20 cycles. Gas-phase product analysis shows that more than 97% of the H₂ originates from water splitting. The results clarify the nature of the active sites in Cu/ZIF-8-derived carbon and their contribution to plasma-catalytic water splitting. Download: Download high-res image (169KB) Download: Download full-size image
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高影响因子
ACS Catalysis
·
2026
·
IF 13.6
Shi Zhanghan,Duan Fangyu,Liu Yafei,Zhang Xianwang,Song Guoquan,Yang Xiaomeng,Ma Qianli,Zhang Zongwu,Wu Dan,Xu Chunbao,Zhang Yongsheng
Cascade catalytic upgrading of biomass-derived furanic compounds to high-value cyclopentanone (CPO) and cyclopentanol (CPL) over metal–acid bifunctional catalysts has attracted considerable attention in sustainable chemistry. However, conventional bifunctional catalysts exhibit insufficient synergistic effects, primarily due to the lack of flexibility in tuning the ratio of acidic to hydrogenative active sites. Herein, we demonstrate that halogen (Br and Cl) modification of supported Cu catalysts significantly enhances both activity and selectivity in the aqueous-phase hydrogenative rearrangement of furfuryl alcohol (FOL), achieving a CPO yield of 94.4% and a CPL yield of 94.6%, respectively. Extensive characterizations reveal that the electronegative Br and Cl adatoms effectively modulate the electronic state of Cu nanoparticles, facilitating the formation of Lewis acidic Cu + sites on the catalyst surface. Mechanistic investigations disclose that Cu + sites mediate the rearrangement of FOL to 4-hydroxy-2-cyclopentenone (4-HCP), while adjacent Cu 0 sites catalyze the hydrogenation of 4-HCP to CPO, followed by its subsequent hydrogenation to CPL. Different binding strengths between Cu and halogens (I > Br > Cl) allow the regulation of the Cu + /Cu 0 ratio on the Cu surface, which in turn provides an effective way to control the reaction pathway. The developed halogen modification strategy not only offers great potential for the upgrading of biomass-derived furanics to cyclopentane derivatives but also presents a versatile strategy for regulating the surface Lewis acidity of metal catalysts, which is crucial for metal–acid bifunctional catalysis.
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高影响因子
Catalysts
·
2023
·Vol. 13
·期 5
·800
·
IF 3.9
Zhong Xie,Jinpei Hei,Lei Cheng,Jing Li,Xiaojie Yin,Sugang Meng
CO2hydrogenation to methanol was conducted using a set of activated carbon-supported Cu/ZnO/Al2O3catalysts (CCZA) prepared by an incipient wetness impregnation approach. The effect of the Cu/Al ratio on the physicochemical properties of the catalysts, as well as their catalytic performance, were investigated. As Cu/Al ratio increased, the metallic Cu surface area displayed a reducing trend from 6.88 to 4.18 m2∙gcat−1, while the CO2adsorption capacity exhibited an increasing trend. Meanwhile, aluminum content will have an important effect on the catalysts’ reducibility and, thus, on their catalytic performance. The CCZA-2.7-de catalyst demonstrated the highest selectivity to methanol at 83.75% due to the excellent distribution and synergistic effect of copper and zinc. Although the CO2conversion of CCZA-2.2-de and CCZA-3.5-de exceeded 10%, the CH3OH selectivity was less than 60%, which may be attributed to the larger particle sizes of ZnO and poor interactions in Cu–Zn. The present study offers a novel approach to increase the number of active sites, optimize the activated carbon-aided Cu/ZnO/Al2O3catalyst’s composition, and finally elucidate the mechanism for CO2hydrogenation to methanol.Keywords:CO2hydrogenation;CuO/ZnO/Al2O3catalyst;methanol synthesis;carbon-supported catalyst;thermocatalysis
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高影响因子
Journal of Environmental Chemical Engineering
·
2022
·
IF 7.968
Zibin Pan,Zhengxian Chen,Gary Owens,Zuliang Chen
Biosynthesis strategies are promising methods for the sustainable preparation of nanoparticles because they are less toxic to living organisms and the environment. However, there are still several knowledge gaps concerning the exact mechanisms involved in the biosynthesis of bimetallic composites when used for the removal of arsenic species. Thus, this work focused on the biosynthesis mechanism involved in the formation of a Fe/Cu bimetallic bio-composite (Fe/Cu-OC), and determination of the specific biomolecules in tea extract involved in biosynthesis, and identification of the reactive sites involved in the removal of As(V). FTIR , XPS, GC-MS, and LC-MS analysis of the main components of the tea extract proved that the surface of Fe/Cu-OC contained many different functional groups, including -OH, Fe/Cu-O, and O C-OH, which were mainly associated with theanine and caffeine complexes. SEM and TEM analyses indicated that Fe/Cu-OC had both crystalline and amorphous features with an average particle size of 366 ± 10 nm. A 97 % removal efficiency for As(V) was obtained by Fe/Cu-OC, suggesting that the surface contained numerous reactive sites, including unsaturated Fe and Cu complexes, as well as saturated benzene rings. Moreover, DFT calculations indicated that the Gibbs free energy changes for the preparation of Fe/Cu-OC were < 0, suggesting that in the composites biosynthesis was a thermodynamically favored spontaneous reaction. A biosynthetic mechanism for the formation of Fe/Cu-OC was proposed, involving a series of spontaneous coordination, redox, and organic adsorption reactions.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2022
·
IF 9.224
Lei Xiao,Chaowei Yuan,Peng Chen,Yongyi Liu,Jianping Sheng,Shihan Zhang,Fan Dong,Yanjuan Sun
Due to the intrinsic chemically inert CO2 with the dissociation energy of C═O bond as high as 750 kJ mol–1, low efficiency and selectivity have become the most significant restraints for the practical application of photocatalytic CO2 reduction. Renewing the electronic structure of adsorbed CO2 on the catalyst surface through a rational catalyst design is crucial to achieving performance improvement. Herein, we prepared ZnIn2S4 and Cu-substituted ZnIn2S4 containing both Lewis acid and Lewis base sites as a model system for investigating the activation of CO2 by M–S chemical bonds (M represents a metal site). The Cu–S chemical bond can effectively activate CO2 as a vital electron channel and lower the Gibbs free energy for generating the essential intermediate *COOH. Besides, the Cu0.7-ZnIn2S4 sample displays 74.8% selectivity for reducing CO2 to CO with a rate of 47.2 μmol g–1 h–1, roughly 7.14 times that of ZnIn2S4.
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高影响因子
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