Nano Energy
·
2025
·
IF 17.1
Tong Li,Huiying Yang,Meiyuan Wu,Kelei Huang,Xiangchao Meng,Zizhen Li
Industrial nitrogen fixation processes, such as the Haber-Bosch and Ostwald processes, are energy-intensive and cause environmental issues. Here, a photothermal evaporation catalytic evaporator was constructed using a core-shell Cu/Cu 2 O (Copper/ Copper(I) oxide) catalyst supported on carbon foam (CF) for efficient overall nitrogen fixation under air. The evaporator utilized the localized surface plasmon resonance (LSPR) effect of Cu nanoparticles and the excellent photothermal conversion capability of CF. It could achieve a surface temperature of 362.2°C under full spectrum light intensity of 1500 mW·cm −2 . The gaseous reaction environment generated by this photothermal evaporator overcame the low solubility of conventional photocatalytic N 2 in water and enhanced mass transfer. The Cu/Cu 2 O interface promoted charge separation, and the hot carriers from Cu nanoparticles accelerated the activation of N 2 . Meanwhile, the charge transfer process between the interfaces (Cu 0 -e - →Cu + , O 2- -e - →OV (Oxygen vacancy), Cu + +e - →Cu 0 , O 2 filled OV) made it possible to ensure the structural integrity throughout the reaction cycle. Under air conditions, the evaporator yield rate of NH 4 + and NO 3 - reached 691.96 μmol g −1 h −1 and 423.87 μmol g −1 h −1 , respectively, surpassing most reported catalysts. In-situ X-ray photoelectron spectroscopy (XPS) and Density functional theory (DFT) calculations revealed that the interface of Cu/Cu 2 O facilitated electron transfer to N 2 , weakening the N N bond and lowering reaction barriers. This work demonstrated a synergistic photothermal-evaporation strategy for efficient nitrogen fixation, providing a sustainable pathway for overall nitrogen fixation in air.
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RSC Advances
·
2024
·Vol. 14
·期 48
·35993-36004
·
IF 3.9
Jinlong Zhong,Xue feng Mao,Guanyu Wang,Heng Li,Junfang Li,Sijian Qu,Jianwei Zhao
Non-homogeneous ozone-catalyzed oxidation technology is one of the effective ways of treating wastewater, the core of which lies in the development of efficient ozone oxidation catalysts. This work proposes the design and synthesis of an efficient Cu/Mn/Ce multi-metal composite oxide catalyst by metal salt precursor mixing-direct granulation. The effect of metal doping on the catalyst properties was compared using Density function theory (DFT) calculations, and the Cu/Mn/Ce co-doping showed significant charge accumulation effect with a low ozonolysis energy barrier, which is more favorable for the generation of reactive oxygen species. The successful loading of the main active metal components, such as Mn, Cu, and Ce, was clarified by systematic characterization by X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), scanning electron microscopy (SEM), energy dispersive spectroscopy (EDS) and Brunauer–Emmett–Teller's test (BET), and the chemical oxygen demand (COD) removal could reach more than 60% for the simulated wastewater. The electron paramagnetic resonance (EPR) characterization clarified that the degradation of organic pollutants was mainly dominated by the combination of single-linear oxygen and superoxide radicals in the catalytic process, and the possible catalytic oxidation mechanism was proposed. This work advances the development of non-homogeneous ozone oxidation technology.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Wanfeng Xiong,Duanhui Si,Jundong Yi,Yuanbiao Huang,Hongfang Li,Rong Cao
Multicomponent heterogeneous catalysts present excellent catalytic performance attributed to the synergistic effect of multi-sites. Nevertheless, identifying the composition of the multi-sites and exploring the synergistic catalytic mechanisms for the multiple active sites in electrocatalytic CO 2 reduction reaction (CO 2 RR) still lack intensive study. This work regulates the chemical composition of Cu-based nanoreactors readily by adjusting the geometrical morphology of metal-organic frameworks precursor. The obtained cuboctahedron nanoreactor containing Cu-N 4 /Cu 2 O/Cu multiple active sites exhibits excellent CO 2 RR selectivity towards deep reduction product (80%) with high current density. Moreover, the tandem catalytic mechanism of multicomponent active sites has been studied intensively. The CO 2 molecule is firstly reduced in Cu-N 4 sites to form CO and then the CO is transfered to Cu 2 O/Cu sites for further deep reduction. The high concentration of CO provided by Cu-N 4 sites decreases the free energy of rate-determining step for CH 4 products in Cu 2 O sites. This work provides a promising direction for designing and synthesizing multicomponent Cu-based tandem catalysts to access high efficiency and selectivity in the electrocatalytic CO 2 reduction reaction.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Yuanli Li,Chunqiang Zhuang,Shi Qiu,Junfeng Gao,Quan Zhou,Zaicheng Sun,Zhenhui Kang,Xiaodong Han
Metal halide perovskites with broad optical absorption and long carrier lifetime are considered as ideal photocatalysts. However, their poor stability in water greatly impedes their application in photocatalytic H 2 evolution because they lose their crystalline structure in water. Herein, we proclaim a new class of photocatalysts: all-inorganic Cs-Cu-Cl perovskite quantum dots (QDs). It exhibits a high photocatalytic hydrogen production rate of ∼ 3.1 mmol/g/h without any cocatalyst under AM 1.5-G solar irradiation (100 mW/cm 2 ). Especially, it remains the high activity for up to 330 h without apparent deterioration of the hydrogen production rate. Density functional theory (DFT) calculations reveal that the Cu site works as the electron and proton absorption sites as the H 2 production active center. To our best knowledge, there is no report of metal halide perovskites as water-stable photocatalysts. This work opens an innovative way for guiding the exploration of metal halide perovskites photocatalysts for stable photocatalytic H 2 evolution.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2025
·
IF 21.1
Zichen Song,Xinxin Zhang,Jianqiu Zhu,Xiaolei Wang,Wenqian Wang,Xiangbo Ma,Jiantao Fu,Jian-Qiang Wang,Guiling Wang,Zhiyu Ren,Honggang Fu
While copper complexes intrinsically provide Cu sites for electrocatalytic CO 2 reduction (ECR), their efficacy toward multicarbon products (C 2+ ) remains fundamentally limited by the operational instability of reactive Cu valence states and the inability to synchronously optimize *CO intermediate generation and C-C coupling within symmetric coordination environments. Herein, we judiciously design a single-crystal N, O co-coordinated copper complex (Cu(ICA) 2 ) featuring asymmetric N 2 -Cu-O 2 centers that precisely modulate the electronic structure and local adsorption environment. The Cu-N bonds stabilize partially reduced Cu δ⁺ sites while weakening Cu-O interactions, thus balancing structural integrity with catalytic reactivity. This asymmetric dual-site coordination concurrently hosts distinct *CO intermediates (atop-adsorbed *CO at Cu sites and bridge-adsorbed *CO at Cu-N sites), enabling cooperative C-C coupling into C 2 products. The catalyst achieves a record 69.2 % Faradaic efficiency for C 2 products at 400 mA cm −2 and 57.4 % for C 2 H 4 at 500 mA cm −2 in 1.0 M KOH, rivaling the state-of-the-art Cu-based complexes. In situ characterization and DFT calculations mechanistically corroborate that bridge-adsorbed *CO at Cu-N sites drives energetically favorable hydrogenation and C-C coupling pathways. This work establishes a coordination-asymmetry design principle for constructing robust molecular catalysts capable of efficient CO 2 -to-C 2+ conversion.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Hui Su,Shaojia Song,Songsong Li,Yangqin Gao,Lei Ge,Weiyu Song,Tianyi Ma,Jian Liu
Rational design of low-cost and efficient electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is imperative for renewable energy conversion. Herein, for the first time, a facile strategy is developed to synthesize M (M = Fe, Cu, Zn, Mo) doped bimetallic sulfide heterostructure Ni 3 S 2 /Co 3 S 4 electrocatalysts. The as-prepared bifunctional Cu-Ni 3 S 2 /Co 3 S 4 electrode exhibits excellent electrocatalytic activity for HER and OER in 1 M KOH electrolyte, and it requires only an overpotential of 79 mV (150 mV) to deliver 10 mA cm −2 (20 mA cm -2 ) current density for HER process. Moreover, it shows a considerable low cell voltage of 1.49 V at the current density of 10 mA cm -2 in a two-electrode configuration which is far surpassing most of the reported bifunctional metal sulfides. Meanwhile, besides increasing the specific surface area of the electrocatalyst by optimizing the microstructure, the introduction of Cu cation could also stimulate the formation of high-valent Ni/Co sites, which can be verified by XPS technique. Density function theory calculations demonstrate that the Cu-doping boosts the formation of high valent Co sites and enhances the charge transfer performance of Ni and Co species, thus promotes intrinsic catalytic activity through modulating the d-band center of Co and reducing the adsorption energy of H and O-containing intermediates (H*, OH*, OOH*) on the surface of the catalyst. This work suggests the importance of exploitation of transition metal ion-doping for promoting the electrocatalytic activity of bimetallic sulfides.
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Matter
·
2025
·
IF 17.5
Bohan Li,Yongsheng Sun,Yuzhen Wang,Jiance Jin,Kai Han,Yan Xu,Zhiguo Xia
Highly transparent and large-area scintillator film is highly desirable for next-generation X-ray imaging and detection. Herein, we develop a rapid and in situ synthesis strategy to fabricate polymer scintillator film composed of (C 14 H 15 P) 4 Cu 4 I 4 glassy cluster gel (M1-GCG). The large-area M1-GCG film of 20 × 12 cm was obtained by in situ UV photopolymerization within 30 s, showing ∼90% transmittance in the broad spectral region of 400–1,000 nm, in which Cu(I) iodide clusters coordinated by phosphine ligands are generated as a glassy form in the polymer network structure and uniformly distributed under supramolecular interactions, as the polymer monomer is polymerized and cross-linked under ultraviolet light. We develop a brand-new chemical synthesis route toward polymer-based composite scintillator film, and the M1-GCG film with high transparency and scintillation properties, as well as high-resolution X-ray imaging ability, shows extraordinary potential for large-area medical imaging and industrial non-destructive detection.
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Advanced Healthcare Materials
·
2025
·
IF 9.6
Xianyu Zhu,Lingli Gao,Yanbo Zheng,Peng Fei Zhao,Hanrui Wei,Ruixue Liu,Liping Zhao,Junyi Zhang,Qi Sun,Lingling Zheng,Han Lv,JiGang Yang,Jianhua Gong,Zhenchang Wang
Poor prognosis and chemotherapy response stem from difficulties in precise targeting and the lack of effective synergistic treatments. Nanozymes show promising potential in tumor chemodynamic therapy (CDT) by catalyzing hydrogen peroxide (H₂O₂) decomposition and glutathione depletion in the tumor microenvironment (TME). However, integrating precise chemotherapy targeting with CDT remains challenging. In this study, a porous Fe/Cu bimetallic nanozyme carrier (FeCuNPs) is developed for co-loading with the humanized 3F8 anti-GD2 disialoganglioside antibody (3F8) and the novel pyridazinone-based chemotherapeutic agent (IMB), forming a nanoreactor (3F8@FeCuNPs@IMB) for targeted chemotherapy and CDT. The nanoreactor responds specifically to the acidic TME as a primary insurance, allowing for the controlled release of IMB at the tumor site. The targeting antibody 3F8 coating on the surface of the nanozyme carrier acts as a secondary insurance, minimizing chemotherapy drug leakage during the delivery process and ensuring precise targeting for effective chemotherapy. Furthermore, FeCuNPs act as peroxidase-like (POD) and glutathione oxidase-like (GSHOX) enzymes, catalyzing hydroxyl radical (•OH) generation and depleting excess GSH, enhancing CDT. The results in vitro and in vivo indicate that the dual insurance designed 3F8@FeCuNPs@IMB offers a promising prospect for a targeted, precise, and effective combination of chemotherapy and CDT against melanoma.
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PubMed
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Ping Li,Huanhuan Wu,Chengming Zhang,Quangui Liang,Huihui Ding,Haibao Zhu,Jun Ma,Xiang Li,Shuangshuang Huai,Congliang Cheng,Xiufang Wang
The lack of active sites and the low availability of photoelectrons severely limit the photocatalytic reduction of nitrogen to ammonia in semiconductor materials. Here, we successfully designed a BiOBr/O v -TiO 2 -Cu heterojunction catalyst toward N 2 fixation into NH 3 . The optimized BiOBr/O v -TiO 2 -Cu heterojunction has a promising photocatalytic performance and stability with the highest NH 3 yield of 259.82 μmol·g −1 ·h −1 . The combination of detailed theoretical simulation calculations and comprehensive characterizations indicates the BiOBr/O v -TiO 2 -Cu heterojunction with oxygen vacancy (O v ) stabilized Cu nanoparticles (NPs) as active sites can effectively adsorb and activate N 2 molecules. The close contact between BiOBr and Ov-TiO 2 elevates the quick transmission of photogenerated electrons at the interface and the enrichment on Cu NPs. This work not only provides an efficient photocatalyst for the N 2 reduction, but also supplies theoretical support for identifying the active sites and charge transfer kinetics of the nitrogen reduction reaction.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2024
·
IF 5.8
Yanke Zhang,Chi Zhang,Wei Chen,Zhengchun Liu
The detection of glucose in beverages is crucial for dietary management and healthcare. Excessive sugar consumption can lead to severe conditions, such as obesity, diabetes, cardiovascular diseases, and cancer. In this study, Cu-embedded laser-induced graphene (Cu/LIG) materials were fabricated for non-enzymatic glucose detection using a simple, direct, and cost-effective laser-patterning method on a Cu 2+ /ethyl-cellulose/polyimide membrane. The experimental results showed that the Cu/LIG electrode exhibited lower charge transfer resistance and a distinct diffusion process compared to the LIG electrode. This improvement can be attributed to the optimized graphene formation achieved by employing ethyl-cellulose (EC) and CuCl 2 as combustion promoters. Under optimal conditions, Cu/LIG-600 demonstrated excellent electrocatalytic activity for glucose oxidation, with a low response concentration (5 μM), fast response time (2.0 s), and detection ranges of 0.005–0.525 mM (I-t) and 0.5–4.0 mM (CV). Moreover, the sensor exhibited high selectivity, stability (retaining over 90 % activity after 28 days), and satisfactory recovery rates for spiked glucose in Cola, Sprite, Black Tea, and sugarless Soda Water, indicating its potential for non-enzymatic glucose detection in beverages.
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2021
·
IF 5.816
Xianglei Liu,Chuang Bao,Zhonghui Zhu,Hangbin Zheng,Chao Song,Qiao Xu
Methanol steam reforming (MSR) is considered as an effective method for hydrogen storage and generating high-quality hydrogen for fuel cells. In this work, mesoporous Cu/TiO 2 –CeO 2 catalysts are proposed to achieve efficient MSR based on synergetic effects of thermal and photon energies . Optimal Ti/Ce molar ratio is found to be 2:1, for which excellent methanol conversion of 100% and extremely low CO selectivity of 2.2% are achieved for thermal catalysis. Further applying UV light (280–400 nm) irradiation while keeping the same temperature, the hydrogen production rate is enhanced to be 78.8 mmol/h/g from 58.6 mmol/h/g. The underlying mechanism is attributed to photogenerated electron hole pairs promoting the REDOX reaction of intermediate product methyl formate based on in situ diffuse reflectance infrared fourier transform spectra (DRIFTS). This work provides a new method to enhance methanol steam reforming performance via thermo-photo synergic effects, and paves a way for the development of direct solar driven MSR techniques.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Linyue Zhang,Jiewen Deng,Jieli Ou,Gaofeng Zhou,Yongsheng Fu,Yiqing Liu
In this paper, it was found that boric acid (BA) could improve the degradation of rhodamine B (RhB) by Cu(II)-activated peroxymonosulfate (PMS). At pH 8.5, the addition of BA could stabilize pH and generate the highly active complexes with Cu(II), which could accelerate the reduction of Cu(II) by PMS. The formed Cu(I) could activate PMS to form sulfate radical (SO 4 – ) and/or be oxidized to Cu(III). According to the results on radical scavenging experiments, SO 4 – and Cu(III) both participated in the degradation of RhB in BA/Cu(II)/PMS system. Because the binding ability of BA with Cu(II) is pH-dependent, the promotion effect of BA in Cu(II)/PMS process occurred only under weakly alkaline conditions. The presence of HCO 3 – and natural organic matter (NOM) both had an inhibition effect on RhB degradation in BA/Cu(II)/PMS system, while Cl – could promote the removal of RhB. This study provides a new idea to enhance PMS activation by Cu(II).
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