Nature Communications
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2025
·Vol. 16
·期 1
·1-11
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IF 15.7
Wang Yi,Wang Shuo,Fu Yunfan,Sang Jiaqi,Wei Pengfei,Li Rongtan,Gao Dunfeng,Wang Guoxiong,Bao Xinhe
Renewable energy-driven electrocatalytic nitrate reduction reaction presents a low-carbon and sustainable route for ammonia synthesis under mild conditions. Yet, the practical application of this process is currently hindered by unsatisfactory electrocatalytic activity and long-term stability. Herein we achieve high-rate ammonia electrosynthesis using a stable amorphous/crystalline dual-phase Cu catalyst. The ammonia partial current density and formation rate reach 3.33 ± 0.005 A cm −2 and 15.5 ± 0.02 mmol h −1 cm −2 at a low cell voltage of 2.6 ± 0.01 V, respectively. Remarkably, the dual-phase Cu catalyst can maintain stable ammonia production with a Faradaic efficiency of around 90% at a high current density of 1.5 A cm −2 for up to 300 h. A scale-up demonstration with an electrode size of 100 cm 2 achieves an ammonia formation rate as high as 11.9 ± 0.5 g h −1 at a total current of 160 A. The impressive electrocatalytic performance is ascribed to the presence of stable amorphous Cu domains which promote the adsorption and hydrogenation of nitrogen-containing intermediates, thus improving reaction kinetics for ammonia formation. This work underscores the importance of stabilizing metastable amorphous structures for improving electrocatalytic reactivity and long-term stability.
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TRANSITION METAL CHEMISTRY
·
2024
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IF 1.6
Han Tianhang,Yao Kaisheng,Wang Zixu,Li Han,Zhao Haili
Nitroaromatic compounds are common toxic matters discharged as wastewater in varied industries. Reducing them into corresponding aromatic amines can not only decrease their contamination but also obtain value-added products, in which the preparation of catalysts with superior properties is the key. Herein, the spherical Cu-Ag architectures (ATs) are constructed via a two-step wet chemical method. First, the Cu microspheres are fabricated with the assistance of polyvinylpyrrolidone (PVP) in the mixed solution of ethylene glycol (EG) and water. Then, using them as templates, the spherical Cu-Ag ATs can be grown and constructed. The as-obtained Cu-Ag ATs have the spherical outlines assembled by many nanoparticles. The sliced Cu-Ag ATs show hollow structures and many nanothorns grow from the center to the around, combining the roughly spherical shell to build up the Cu-Ag ATs. In the reduction reaction of p -nitrophenol and p -nitroaniline, the spherical Cu-Ag ATs all exhibit excellent catalytic activities. Within 85 s and 80 s, the p -nitrophenol and p -nitroaniline can be converted completely. The prepared Cu-Ag ATs are expected to have potentials in other fields, such as electronics, sensors and so on. Graphical abstract The hierarchical Cu-Ag architectures are constructed successfully through a two-step wet chemical method, in which the rough Cu microspheres are first fabricated in aqueous EG solution, and are used as templates to direct the growth of Cu-Ag architectures. In both reduction of p -nitrophenol and p -nitroaniline, the Cu-Ag architectures exhibit high catalytic activities.
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DALTON TRANSACTIONS
·
2020
·Vol. 49
·期 34
·11851-11858
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IF 4.174
Shuhua Cao,Xuezhao Li,Yong Gao,Fahui Li,Kaoxue Li,Xuanxuan Cao,Yiwen Dai,Lirong Mao,Shanshan Wang,Xishi Tai
A bimetallic Cu(II) complex as a novel antitumor chemodynamic therapy agent with glutathione (GSH) depletion properties is successfully synthesized and well characterized. In tumor cells, the Cu2+ ions of the complex are reduced to Cu+ ions by GSH and then catalyzed by the overexpressed H2O2 to generate highly cytotoxic hydroxyl radicals (˙OH) that kill cancer cells. The complex is quickly taken up by cancer cells and distributed in multiple organelles including mitochondria and the nucleus. The complex demonstrates good cytotoxicity toward various cancer cell lines. However, its toxicity toward normal cells is significantly lower than that toward cancer cells due to the limited expression of H2O2. In addition, the complex could arrest the cell cycle of the G0/G1 phase, thereby inducing apoptosis rather than necrosis.
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Nature Communications
·
2025
·Vol. 16
·期 1
·1-18
·
IF 15.7
Shen Yan,Fang Nan,Liu Xinru,Ling Yu,Su Yuming,Tan Tian,Chen Feng,Lin He,Zhao Boxuan,Wang Jin,Si Duanhui,Xie Shunji,Wang Ye,Zhou Da,Zhang Teng,Cao Rong,Wang Cheng
Interphases are critical in electrochemical systems, influencing performance by controlling ion transport and stability. This study explores a metal-organic interphase in the electrocatalytic reduction of CO 2 (CO 2 RR) on Cu, extending the concept of interphases to CO 2 conversion. Investigating organic modifications on CuO x , we discover metal-organic interphases over 10 nm thick in highly ethanol-selective systems, contrary to the expected monolayer adsorption. Using an automated platform, 1080 CO 2 RR experiments with 180 molecular modifiers identify functional groups affecting selectivity for ethanol and multi-carbon (C 2+ ) products. We find that these modifiers consistently produce metal-organic interphases on the Cu or CuO x surface. These interphases modulate Cu coordination, CO 2 RR intermediates, and interfacial water configuration, significantly improving electrocatalytic performance. Testing across 11 CuO x -based catalysts validates this approach, culminating in the development of two electrocatalysts that achieve ~80% faradaic efficiency for C 2+ products with ethanol partial current densities up to 328 and 507 mA cm −2 . This study highlights the pivotal role of interphases in CO 2 RR, advancing CO 2 conversion technologies.
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Energies
·
2024
·Vol. 17
·期 6
·1449
·
IF 3
Qiong Li,Yu Wang,Ganghui Wei,Xiaorong Fang,Ni Lan,Yonggang Zhao,Qiming Liu,Shumei Lin,Deyan He
The preparation of composite carbon nanomaterials is one of the methods for improving the electrochemical performance of carbon-based electrode materials for supercapacitors. However, traditional preparation methods are complicated and time-consuming, and the binder also leads to an increase in impedance and a decrease in specific capacitance. Therefore, in this work, we reduced Ni-Cu nanoparticles on the surface of nitrogen-doped carbon nanofibers (CNFs) by employing an electrostatic spinning method combined with pre-oxidation and annealing treatments. At the same time, Ni-Cu nanoparticles were vulcanized to Ni–Cu–S nanoparticles without destroying the structure of the CNFs. The area-specific capacitance of the CNFs/Ni–Cu–S–300 electrode reaches 1208 mF cm−2at a current density of 1 mA cm−2, and the electrode has a good cycling stability with a capacitance retention rate of 76.5% after 5000 cycles. As a self-supporting electrode, this electrode can avoid the problem of the poor adhesion of electrode materials and the low utilization of active materials due to the inactivity of the binder and conductive agent in conventional collector electrodes, so it has excellent potential for application.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2024
·
IF 9.4
Mengchen Wu,Yang Yang,Jing Zhao,Rui Liu
In CO 2 electroreduction, mutative intermediates and the challenging C C coupling necessitate the spatial interplay between active sites and through dynamically optimizing configurations. Herein, we anchor ethylenediaminetetraacetic acid (EDTA)-bonded Cu x+ /Bi 3+ pair within UiO-66 for a spontaneous spatial-optimizing CO 2 -to-C 2 H 4 electroreduction. Ab initio molecular dynamic (AIMD) simulation visualizes that such metal pair adaptively interacts with intermediates. Density functional theory (DFT) elicits the componential synergy, in which an upshift d-band of Cu activates CO 2 being protonated into *COOH while Bi site stabilizes oxygenated dimers for deep hydrogenation. The dynamic feature of such pair affords large freedom for sorption and migration of various intermediates, which consequently bestows UiO-66-EDTA/CuBi a maximal FE C 2 H 4 of 47 % and a total current density over 100 mA cm −2 in the flow cell.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Xingyue Yang,Lei Wang,Shijie Zhou,Shilong Zhang,Yongfang Xu,Yujie Bian,Zhaowei Tian,Yusen Yang,Min Wei
Liquid organic hydrogen carriers (LOHC), which involve reversible catalytic hydrogenation/dehydrogenation cycles, have attracted considerable attention. This study investigates Cu/CuAlO x catalysts with unique Cu 0 –Cu + interfacial sites, which are prepared via structural topological transformation of layered double hydroxide (LDH) precursors. The optimized Cu/CuAlO x catalysts exhibit exceptional catalytic activity in 1,2,3,4-tetrahydroquinoline (THQ) dehydrogenation, achieving a complete conversion of THQ within 1.5 h and a turnover frequency (TOF) value amounts to 19.94 h −1 at 150 °C, which stands at the highest echelon compared with previously reported heterogeneous catalysts. Furthermore, the catalyst also exhibits excellent performance in quinoline hydrogenation (yield >99 %) after 6 h at 60 °C, and the TOF value reaches up to 7.01 h −1 . A comprehensive investigation based on XPS, TEM and XAFS verifies the dual active states Cu 0 and Cu + sites coexisting on nanoparticle surfaces. Both experimental studies ( in situ DRIFTS and XPS) and DFT calculations reveal the pivotal role of the Cu 0 − Cu + synergistic effect in dictating catalytic behavior: the Cu + species preferentially adsorb and activate the N − H bonds and C − H bonds in N-heterocycles; Whereas the Cu 0 site facilitates efficient reassociation of surface adsorbed H atoms and product desorption (H 2 ). This work exhibits substantial potential for implementation in hydrogen storage technologies, offering a viable pathway towards efficient LOHC utilization in clean energy systems.
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JOURNAL OF THE ENERGY INSTITUTE
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2024
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IF 5.6
Zheng Bo,Mengyu Cao,Yaolin Wang,Jianhua Yan,Kefa Cen,Xin Tu
Plasma catalytic CO 2 hydrogenation has emerged as a promising approach for converting CO 2 into valuable chemicals such as CO, offering a potential solution to mitigate greenhouse gas emissions. In this study, we investigate the synergistic effect between plasma and a Cu/Ti 3 C 2 T x MXene catalyst for CO 2 hydrogenation via the reverse water gas shift (RWGS) reaction in a dielectric barrier discharge (DBD) reactor. Our findings reveal a significant enhancement in CO 2 conversion (33.1%) and CO yield (31.9%) when using the Cu/Ti 3 C 2 T x catalyst compared to plasma alone or with a Ti 3 C 2 T x foam. Plasma treatment creates unsaturated Ti sites on the Ti 3 C 2 T x surface, dramatically improving CO 2 adsorption and activation, while Cu nanoparticles significantly enhances the activation and dissociation of H 2 molecules on the catalyst surface. These surface adsorbed hydrogen species readily hydrogenate adsorbed CO 2 molecules through the Langmuir-Hinshelwood mechanism. Furthermore, these surface hydrogen species can also participate in the conversion of gas-phase CO 2 molecules through the Eley-Rideal pathway. This work sheds light on the synergistic plasma catalytic mechanism and provide insights for optimizing CO 2 hydrogenation processes using MXene catalysts.
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ACS Catalysis
·
2025
·
IF 13.1
Xiaodong Wen,Qizhi Min,Xiaodong Liu,Gang Zhao,Junyao Wang,Qinshang Xu,Guoshuai Shi,Liming Zhang,Wenhua Zhang,Yude Su
Structural reconstruction─an uncontrollable process that compromises the stability of Cu-based catalysts in electrochemical CO2 reduction (CO2R)─presents a major scientific challenge that has yet to be overcome. In this work, we develop a well-controlled SiO2 encapsulation approach to stabilize Cu-based CO2R electrocatalysts against reconstruction. Using Cu nanowires (CuNWs) as a model platform, we demonstrate that SiO2 encapsulation can significantly suppress Cu reconstruction while retaining ∼95% of the initial CO2R performance over 24-h stability tests at −1.15 V vs reversible hydrogen electrode (VRHE). In contrast, unencapsulated CuNWs exhibit severe structural deterioration with attenuated CO2R activity under identical testing conditions. In situ Raman studies and density functional theory (DFT) calculations reveal that the antireconstruction effect results from the formation of a robust Cu–O–Si interface that can not only serve as a structural anchor but also contribute to strengthening the Cu–Cu bonding at the exposed Cu active sites during CO2R operation. These results decipher the stabilizing mechanism of SiO2 encapsulation, and provide key insights for designing durable Cu-based CO2R electrocatalysts toward practical applications.
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Energy Storage Materials
·
2025
·
IF 20.2
Siyu Fang,Tiansheng Bai,Jialin Liao,Shuai Zhang,Jiaxian Wang,Funian Mo,Wei Zhai,Zhenglin Hu,Jingyu Lu,Kwun Nam Hui,Lijie Ci,Deping Li
Lithium metal anodes hold the potential for high-energy-density batteries due to their substantial theoretical capacity, but their practical application is hindered by issues such as dendrite growth, poor cycling stability, and safety concerns. This study presents the development of a three-dimensional Li-Si composite alloy anode (Ag@Cu@Li-Si), combining a porous copper scaffold with a lithiophilic silver (Ag) layer and a lithium-silicon (Li-Si) alloy. The Ag@Cu@Li-Si composite demonstrates significant improvements in dendrite suppression, cycling stability, and electrochemical performance. The composite anode exhibits a critical current density of 15 mA cm −2 and over 900 hours of stable operation at 1.0 mA cm −2 in symmetric cells. When integrated into a full cell with a commercial LiFePO 4 cathode, it maintains excellent cycling stability, delivering over 600 cycles with a rate capability of 1.0 C. This study provides valuable insights into the design of lithium metal anodes, highlighting the importance of lithiophilic materials and 3D frameworks for high-performance lithium-metal batteries.
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ACS Sensors
·
2025
·
IF 9.1
Lingli Ji,Jie Sun,Baijing Li,Shuo Cheng,Zhao Zhang,Feng Gao,Jianbo Sun
Accurately detecting hydrogen sulfide in the environment and monitoring its pollution sources are crucial for pollution assessment and personal safety. However, rapid detection is a challenge due to the influence of carrier behavior and surface adsorption states. In this paper, Cu-doped W18O49 nanowires were synthesized by the solvothermal method. The surface field effect phenomenon resulting from doping and H2S adsorption enables a rapid response to H2S with significantly improved responsivity. We characterized the material’s structure and properties by SEM, TEM, and XRD techniques, verified the surface microelectric field effect by combining XPS and field effect device in situ gas sensing characterization, and discussed the sensitive mechanism of hydrogen sulfide.
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ACS Applied Energy Materials
·
2025
·
IF 5.5
Zhengshuai Cao,Mu Li,Li Shan,Mingshang Liu,Wenming Li
SnTe is an environmentally friendly and promising alternative thermoelectric material in contrast to harmful PbTe. However, the long-lasting high lattice thermal conductivity significantly inhibits the further enhancement of the thermoelectric figure of merit ZT. Herein, this study proposed a strategy of solvothermal copper doping to considerably reduce the lattice thermal conductivity by introducing multiscale hierarchical structures. The structural and morphological characterizations indicate that Cu was doped as interstitial atoms and secondary-phase Cu1.80Te. Simultaneously, this study reveals that Cu1.80Te and the SnTe matrix stem from nanoparticles and octahedral structures, respectively. In the sintered bulks, phonon scattering was significantly increased owing to the abundant micro/nanopores, Cu1.80Te nanoprecipitates, grain boundaries of SnTe, and phase boundaries between Cu1.80Te and SnTe. The increased phonon scattering leads to a lattice thermal conductivity of ∼0.36 W m–1 K–1 at 773 K, which is lower than that of pristine SnTe. Benefiting from this substantially decreased thermal conductivity, a ZT value of ∼0.91 was achieved in Sn0.98Cu0.02Te. The enhancement is ∼300% over pristine SnTe. This work provides an effective method to fabricate high-performance energy-effective SnTe-based thermoelectric materials.
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