APPLIED SURFACE SCIENCE
·
2025
·
IF 6.9
Zong Li,Kaili Ni,Yifei Wang,Yuan Rui,Miaohui Wang,Haiping Lin,Peipei Huang,Qing Li
Achieving high activity and selectivity for multi-carbon (C 2+ ) products on copper-based catalysts at ampere-level current densities is important for advancing industrial electrochemical CO 2 reduction reaction (eCO 2 RR). However, oxidative copper species are prone to reduction to metallic copper at high reduction potentials, causing the decline of selectivity and stability for C 2+ products. Herein, we report that Cucurbit[6]uril (CB[6])-modified copper nanoparticles promote eCO 2 RR via stabilizing Cu + sites at ampere-level current densities. The Cu-CB[6]-3 catalyst exhibited the highest C 2+ productivity with a faradaic efficiency of 72.2 ± 1.0 % at a current density of 1.0 A cm −2 , and the corresponding potential was −1.2 V vs. RHE. Detailed systematical spectroscopic analyses revealed that the main reason for boosting the C–C coupling is that the strong coordination interaction and molecular-level confinement of CO 2 and reaction intermediates of CB[6] can not only stabilize Cu + at higher current densities, but also accelerate the reaction kinetics. Simultaneously, the hydrophobic inner cavity and hydrophilic outer surface of CB[6] molecules ensure the smooth progress of eCO 2 RR while suppressing the hydrogen evolution reaction, resulting in high C 2+ selectivity and long-term stability. This work provides an approach to design highly efficient catalysts for industrial eCO 2 RR.
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ACS Omega
·
2025
·
IF 4.3
Chaofan Deng,Chun Cai
Pd–Cu bimetallic catalysts were successfully synthesized for the dehydrogenation of Bisphenol Z (BPZ) by an impregnation-reduction method. The obtained catalyst was studied by XRD, HRTEM, XPS, BET, and NH3-TPD techniques and effectively applied in the highly selective cleavage dehydrogenation of BPZ to give PPP > 99% yield at 270 °C and atmospheric pressure in the solvent-free condition. It was demonstrated that the “synergistic effect” of the bimetallic catalysts could effectively promote the cleavage dehydrogenation reaction. Pd species served as the primary active sites for the adsorption and dissociation of H* and the activation of C–H bonds, while the introduced Cu species accelerated the breaking process of the C–H bond. This catalyst demonstrated remarkable stability and could be reused over ten cycles without obvious decrease both in yield and selectivity. The likely reaction pathway was outlined to elucidate the cleavage dehydrogenation mechanism according to experimental results.
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AICHE JOURNAL
·
2025
·
IF 4
Fei Fan,Dechao Wang,Zengyi Li,Wulong Lu,Jianwei Liu,Xiaoyi Wei,Xu Cheng,Houxiang Sun,Huabing Zhang,Zhiping Chen,Wenwu Zhou
Developing high-performance supported non-precious metal copper-base catalysts for CO 2 hydrogenation is of extreme significance for the successful production of green methanol (CH 3 OH). Herein, Cu/ n Ge-CeO x catalysts ( n = 0, 0.25, 0.5, and 1 wt%) were synthesized via the incipient wetness impregnation method and comprehensively investigated using experiments and DFT calculations. Among all the catalysts, the Cu/0.5Ge-CeO x catalyst exhibited the highest concentration of oxygen vacancies, the smallest Cu grain size, and the most favorable regions for CO 2 adsorption. Compared to the Cu/0Ge-CeO x catalyst, the CH 3 OH yield was significantly improved over the Cu/0.5Ge-CeO x catalyst in the temperature range of 220–260°C under 3 MPa and a gas hourly space velocity of 3000 mL·g cat −1 ·h −1 . Especially at 260°C, the yield sharply increased from 35.23% to 82.21%, and this catalyst maintained high activity for 100 h. This was because the inert pair effect of the introduced Ge promoters induced lattice distortion on the support surface and regulated its microregion electron structures, while simultaneously establishing a highly active interface on the adjacent Cu cluster. This not only enabled an integrated process of in situ activated CO 2 and hydrogenation, but also inhibited the HCOO pathway, lowered the barrier of the rate-controlling step of the RWGS pathway, and reconciled some of its competing branching routes.
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Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hongyang Zhao,Jingying Luo,Zhuojian Li,Shuya Cui,Li Liu,Xin Tong
Manipulating the intrinsic properties of colloidal quantum dots (QDs) offers a promising pathway to achieve efficient solar-driven photoelectrochemical (PEC) hydrogen evolution toward carbon neutrality. In this work, a novel environmentally benign light-harvesting material of silver (Ag) and copper (Cu) co-doped zinc–indium–sulfide/zinc selenide (Zn–In–S/ZnSe) core/shell QDs was developed, wherein the co-dopants establish a synergistic charge transfer pathway of Ag-mediated hole migration to Cu acceptor states in the QDs, thus creating a stabilized donor–acceptor configuration for enhanced charge carrier extraction. As a consequence, the PEC devices fabricated using the optimized Ag, Cu-ZIS/ZnSe QDs delivered a maximum photocurrent density of 8.9 mA cm−2 at 0.6 V versus the reversible hydrogen electrode (vs. RHE) under 1 sun AM 1.5G illumination (100 mW cm−2), representing a 6.4-fold improvement over the undoped ZIS/ZnSe QD PEC systems. Moreover, the fabricated Ag, Cu-ZIS/ZnSe QD-based PEC device exhibited a hydrogen production rate of 105.8 μmol cm−2 h−1 with a faradaic efficiency (FE) of 72.4%, which is 8.5 times higher than the control device based on the undoped QDs. Our work presents a synergistic dopant engineering technique to optimize the charge kinetics of eco-friendly QDs for highly efficient PEC applications, showing great potential for constructing environment-friendly, low-cost and high-efficiency solar energy conversion systems.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ruihong Guo,Yujuan Zhang,Xiutang Zhang,Hong Yang,Tuoping Hu
The development of efficient bifunctional catalysts is the key technology to replace oxygen evolution reaction (OER) with hydrazine oxidation reaction (HzOR) with lower theoretical potential to achieve high efficiency and energy-saving hydrogen production . In this work, the Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite with flower-like array was prepared by two-step electrodeposition coupled pyrolysis method. The electrochemical measurements showed that the driving voltages of the optimal composite for HzOR and hydrogen evolution reaction (HER) are respectively −118 mV and 47 mV at a current density (j) of 10 mA cm −2 . The excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) composite is attributed to the fact that the flower-like structure exposes more active areas and facilitates the diffusion of electrolyte, the strong electron interaction between Co 0·52 Cu 0·48 /Cu and S –C substrate, which can be verified by X-ray photoelectron spectroscopy (XPS), enhances the electrical conductivity , the Co 0·52 Cu 0·48 /Cu heterogeneous interface reduces the water dissociation barrier and facilitates the dehydrogenation kinetics of N 2 H 4 determined by density functional theory (DFT) calculations. Due to the excellent performance of Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V), the overall hydrazine splitting (OHzS) electrolytic cell was constructed with Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) as electrodes. The results showed the voltages required by the cell are 36, 210 and 282 mV at the current density values of 10, 100 and 200 mA cm −2 respectively, showing that Co 0·52 Cu 0·48 /Cu@S–C (−1.3 V) can be used for energy-saving hydrogen production by hydrazine assisted water electrolysis.
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MOLECULES
·
2024
·Vol. 29
·期 16
·3832
·
IF 4.2
Song-Yu Luo,Chun-Mei Zeng,Ping Xu,Ye Ning,Meng-Lin Dong,Wen-Hua Zhang,Guangliang Yu
In this work, we report the synthesis of a new thiosemicarbazone-based drug of N′-(di(pyridin-2-yl)methylene)-4-(thiazol-2-yl)piperazine-1-carbothiohydrazide (HL) featuring a thiazole spectator for efficient coordination with Cu(II) to give [CuCl(L)]2(1) and [Cu(NO3)(L)]2(2). Both1and2exhibit dimeric structures ascribed to the presence of di-2-pyridylketone moieties that demonstrate dual functions of chelation and intermolecular bridging. HL,1, and2are highly toxic against hepatocellular carcinoma cell lines Hep-G2, PLC/PRF/5, and HuH-7 with half maximal inhibitory concentration (IC50) values as low as 3.26 nmol/mL (HL), 2.18 nmol/mL (1), and 2.54 × 10−5nmol/mL (2) for PLC/PRF/5. While the free ligand HLmay elicit its anticancer effect via the sequestration of bio-relevant metal ions (i.e., Fe3+and Cu2+),1and2are also capable of generating cytotoxic reactive oxygen species (ROS) to inhibit cancer cell proliferation. Our preliminary pharmacokinetic studies revealed that oral administration (per os, PO) of HLhas a significantly longer half-lifet1/2of 21.61 ± 9.4 h, nearly doubled as compared with that of the intravenous (i.v.) administration of 11.88 ± 1.66 h, certifying HLas an effective chemotherapeutic drug via PO administration.
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Analytical Methods
·
2025
·
IF 2.6
Shuhuai Li,Yinian Zhu,Xionghui Ma,Chaohai Pang,Rui Chen,Zongqiang Zhu
The amplification of detection signals is an important method for improving the sensitivity of electrochemical detection. This study presents an efficient strategy for preparing electrochemical catalytic materials using a simple self-assembly technique to encapsulate Fe single atoms (Fe–SAs) and Ni single atoms (Ni–SAs) in the Cu-benzene-1,3,5-tricarboxylic acid (Cu-BTC) metal–organic framework to form a Cu-BTC@FeNi–SAs catalytic system. Subsequently, Cu-BTC@FeNi–SAs was modified on the surface of a gold electrode, and sulfadiazine was used as a template to prepare a molecularly imprinted polymer (MIP) on the modified electrode. After eluting sulfadiazine, an MIP was obtained for specifically recognising sulfadiazine. When sulfadiazine was adsorbed by the MIP, a differential pulse voltammetry (DPV) signal occurred in response, thus detecting sulfadiazine. The adoption of Cu-BTC-fixed FeNi–SAs significantly facilitated mass transfer during the reaction, thus improving the DPV response signal. When used to detect sulfadiazine, the sensor had a linear range from 5 × 10−12 to 6000 × 10−12 mol L−1 and a detection limit of 1.14 × 10−12 mol L−1. It also successfully detected sulfadiazine residue in seawater and fish samples with recovery rates between 91.02% and 99.20%.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Xiaohang Sun,Zhengzuo Liu,Shuairen Qian,Kaiqi Nie,Zhengwen Li,Weiming Wan,Binhang Yan
Designing an active Cu/ZnO interface is crucial for efficient catalytic hydrogenation of CO 2 to methanol. In this study, we introduce a straightforward impregnation method to synthesize HKUST-1-derived inverse ZnO x /Cu catalysts. The resulting ZnO x /Cu interface exhibits outstanding methanol space-time yield and selectivity, surpassing conventional Cu/ZnO catalysts synthesized via the co-precipitation and impregnation methods. In situ characterization reveals that small, well-dispersed ZnO x nanoparticles are located on moderately sized Cu nanoparticles, which is attributed to the high specific surface area and ligand coordination of HKUST-1. The inverse ZnO x /Cu structure promotes the formation of reduced ZnO x nanoparticles, which significantly enhance CO 2 and H 2 activation, resulting in increased methanol production. Additionally, the moderate size of Cu nanoparticles minimizes CO* intermediate formation, further enhancing methanol selectivity. This work not only offers valuable insights for the development of new Cu/ZnO catalysts but also provides guidance for the synthesis of inverse metal oxide/metal catalysts for other catalytic systems.
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LANGMUIR
·
2025
·
IF 3.9
Jiao Wang,Yang Yu,Anqi Wang,Chunxu Chen,Shaojun Li,Lei Bai
The efficient activation of the O–O band in persulfate (PDS) with high energy was important and could be achieved by the interface engineering of catalysts. It was discovered that the robust bisphenol A (BPA) degradation could be achieved in the presence of PDS via different mechanisms with steel-wool-shaped Cu–Co3O4 composites obtained via in-situ hydrolysis of cobalt and copper nitrate with zeolitic imidazolate framework-67 after calcination. The calcination temperature at 483 K resulted in abundant oxygen vacancies in Cu–Co3O4 with the amorphous structure, which displayed about a 25-fold higher degradation rate constant (k = 0.385 min–1) than that (0.015 min–1) of Co3O4 for BPA disposal with PDS, possibly via forming the surface-activated complex process. The higher temperature (583 K) treated Cu–Co3O4 could also lead to the fast BPA degradation with the k of 0.670 min–1, which was more than 160-fold higher than the referenced Co3O4 and experienced the radical and nonradical processes, including the HO•, SO4•–, O2•–, and 1O2 as reactive oxygen species. The above difference was possibly due to the amount of oxygen vacancy, the ratio of metal ions with different oxidation states, and the interaction of Cu–O–Co in the composite.
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Chem
·
2024
·
IF 19.1
Xi Cao,Shan Ren,Xue Zhang,Qikui Fan,Qingqing Chen,Jian Yang,Junjie Mao
Cu-based catalysts are boosting electrocatalysts in CO 2 reduction reactions to high-value multicarbon (C 2+ ) products. Because of the unstable Cu + species and the unclear microscopic structure in reactions, Cu-based catalysts still face significant challenges of low selectivity and poor durability at high current density. Herein, we report a thermodynamically driven comproportionation strategy for forming a Cu 0 /Cu + /Cu 0 interface to stabilize Cu + species. When tested in a flow cell containing neutral electrolyte, the sample showed a high C 2+ products Faradaic efficiency (FE C2+ ) of 92.3% at a partial current density of 276.9 mA cm −2 . In a membrane electrode assembly, the sample achieved a 90.1% FE C2+ and maintained continuous operation for over 50 h at industrial current density. Further investigation demonstrates outstanding FE C2+ of >80% at a large industrial current of 10 A. Mechanism studies reveal that the Cu 0 /Cu + /Cu 0 interface lowers the energy barrier for C–C coupling in the reaction, thus facilitating the conversion of CO 2 to C 2+ products.
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Advanced Fiber Materials
·
2024
·Vol. 6
·期 2
·444-457
·
IF 17.2
Xiao Yuanxiang,Jiang Jingjing,Cai Rui,Fu Jiajia,Xiang Shuangfei,Zhao Shujun,Fu Feiya,Diao Hongyan,Liu Xiangdong
Unpredictable pandemics are likely to pose a significant global threat in the future, and biologically protective textiles will play critical roles in controlling the spread of pathogens during outbreaks. Herein, we present a novel metal–organic framework (MOF) composed of repeating units of a Cu(II)/(L-Cys) 2 complex formed through coordination bonds between Cu(II) and L-Cys, while being interconnected by ionic bonds involving Cu(II) and the carboxylate group of L-Cys. After covalently embedding the MOF nanofibers onto cotton fiber surfaces, the resulting fabrics exhibit remarkable virucidal and antibacterial capabilities. Remarkably, even after 200 friction or 50 laundering cycles, the high antiviral ability to inactivate all phi- × 174 within 10 min was maintained, and the bacterial reduction rate against E. coli and S. aureus remained nearly at 100%. The remarkable virucidal effect of the L-Cys@Cu MOF structure is elucidated through a series of α-amylase denaturation simulation tests, providing the first experimental demonstration of the antiviral mechanism, whereby MOF nanofibers induce protein denaturation to inactivate viruses. Moreover, cytotoxicity assessments confirm that the fabrics adorned with MOF nanofibers are safe for human skin. These advantages are promising for the development of protective textiles, highlighting the great potential of nanoscience in combating pandemics. Graphical Abstract
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ELECTROCHIMICA ACTA
·
2024
·
IF 5.5
Jinjing Du,Yu Zhou,Xinhai Liu,Xinxin Cui,Xuan Zhang,Bin Wang,Xiao Feng,Jun Zhu,Heng Zuo,Qian Li,Xihong He,Ping Hu
The development of a hydrogen evolution catalyst with both catalytic activity and stability is critical for hydrogen production from electrolytic water. Herein, a V-based porous alloy was prepared via high-energy ball milling and solid-state sintering. Then, the V-based porous alloy was modified with a Ni-Cu-Mo ternary alloy coating by direct current electrodeposition to obtain a composite hydrogen evolution cathode with high hydrogen evolution activity. The substrate has a certain hydrogen storage capacity combined with a high-activity Ni-Cu-Mo coating. The composite hydrogen evolution cathode exhibited high electrocatalytic activity toward the HER. It can afford a lower overpotential of 93 mV and a smaller Tafel slope of 97.4 mV/dec with a current density of 10 mA/cm 2 in 1.0 M KOH. The composite hydrogen evolution cathode demonstrated outstanding stability after 2000 cycles and good durability after intermittent electrolysis for 20 h. Hydrogen protons can protect the components of the cathode composite from dissolution during discontinuous constant potential electrolysis. The composite hydrogen evolution cathode also exhibited a strong catalytic capacity for hydrogen evolution during intermittent electrolysis under alkaline conditions.
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