Controlled Growth Interface of Charge Transfer Salts of Nickel-7,7,8,8-Tetracyanoquinodimethane on Surface of Graphdiyne
Controlled Growth Interface of Charge Transfer Salts of Nickel-7,7,8,8-Tetracyanoquinodimethane on Surface of Graphdiyne
- Research Article
5
- 10.1002/ange.202216397
- Jan 10, 2023
- Angewandte Chemie
Abstract Vacancies can significantly affect the performance of metal oxide materials. Here, a gradient graphdiyne (GDY) induced Cu/O‐dual‐vacancies abundant Cu0.95V2O5@GDY heterostructure material has been prepared as a competitive fast‐charging anode material. Cu0.95V2O5 self‐catalyzes the growth of gradient GDY with rich alkyne‐alkene complex in the inner layer and rich alkyne bonds in the outer layer, leading to the formation of Cu and O vacancies in Cu0.95V2O5. The synergistic effect of vacancies and gradient GDY results in the electron redistribution at the hetero‐interface to drive the generation of a built‐in electric field. Thus, the Li‐ion transport kinetics, electrochemical reaction reversibility and Li storage sites of Cu0.95V2O5 are greatly enhanced. The Cu0.95V2O5@GDY anodes show excellent fast‐charging performance with high capacities and negligible capacity decay for 10 000 cycles and 20 000 cycles at extremely high current densities of 5 A g−1 and 10 A g−1, respectively. Over 30 % of capacity can be delivered in 35 seconds.
- Research Article
- 10.1039/d5ay01205h
- Jan 1, 2025
- Analytical methods : advancing methods and applications
This review aims to critically examine the development, capabilities, and future prospects of nano-electrochemical sensors as a next-generation solution for the rapid and accurate detection of crop viruses. The motivation stems from the urgent need to overcome the shortcomings of conventional diagnostic tools-such as ELISA and PCR-which, while accurate, suffer from drawbacks in speed, portability, and adaptability to evolving viral threats. We first introduce the fundamental architecture and working principles of electrochemical biosensors, emphasizing key transduction mechanisms including amperometry, voltammetry, and electrochemical impedance spectroscopy. A major focus is placed on the role of nanomaterials-such as gold nanoparticles, carbon-based nanostructures, quantum dots, metal-organic frameworks (MOFs), and MXenes-in enhancing sensor performance through improved surface area, electron transfer, and bioreceptor immobilization. Real-world applications are highlighted through recent advances in detecting agriculturally important viruses like tobacco mosaic virus, plum pox virus, and Citrus tristeza virus, with emphasis on sensitivity, selectivity, and response time. The review also explores current limitations, such as sensor reproducibility, field stability, and biofouling, as well as emerging directions including multiplexed detection systems and integration with Internet of Things (IoT) networks and artificial intelligence (AI) platforms for real-time crop health monitoring. By synthesizing technological advances and outlining actionable research pathways, this review underscores the transformative potential of nano-electrochemical sensors in plant virology and precision agriculture.
- Research Article
- 10.1002/smll.202501867
- Apr 14, 2025
- Small (Weinheim an der Bergstrasse, Germany)
The birth of metal atom catalysts marked a new historical stage in the field of catalysis, allowing scientists to better understand the science of catalysis at the atomic level. On the basis of anchoring independent metal atoms, bimetal dysprosium-copper atoms are successfully anchored on graphdiyne (DyCu/GDY). Dy and Cu metal atoms are selectively anchored in triangular holes of GDY and stabilized by non-integer charge transfer and the confined space effect between the metals and GDY. The dynamic charge-transfer equilibrium caused by the inherent non-integer charge transfer between GDY and metal atoms produces sustained high activity, inducing a redistribution of surface charge. This result shows that the non-integer charge transfer strongly promotes the adsorption activation of CO2 and the desorption of the reaction intermediates, realizing the unpredictable selectivity and activity of CO2 conversion in the process of artificial photosynthesis, where the selectivity and yield of CO are 98% and 279µmol gcat. -1h-1, respectively.
- Research Article
- 10.1002/adfm.202519797
- Oct 7, 2025
- Advanced Functional Materials
Abstract Environmentally sustainable electrocatalytic nitrate reduction (NO3RR) is a very promising method for the synthesis of ammonia at room temperature via the complex eight‐electron/nine‐proton transfer mechanism. Herein, the local electric field‐assisted electrochemical NO3RR process is proposed to identify the origin of catalytic activity and charge transfer kinetics resulting from different morphologies of the electrocatalyst. Accordingly, Ni(TCNQ)2/NF nanorods (NRs) and nanotips (NTs) are fabricated on Ni foam as electrocatalysts for the NO3RR. The Ni(TCNQ)2/NF NTs exhibits an impressive ammonia yield of up to 11286.9 µg h−1 cm−2 and a Faradaic efficiency (FE) of 83.7% at −1.0 V versus RHE, representing nearly a 2.2‐fold increase in yield compared to the Ni(TCNQ)2/NF NRs. This greater performance is attributed to the local enhanced electric field (LEEF) generated at the tip‐like Ni(TCNQ)2/NF NTs. Furthermore, a Zn–NO3− battery is developed here, and Ni(TCNQ)2/NF NTs shows a maximum power density of 2.15 mW cm−2. Experimental and computational findings demonstrate that the geometric and electrical properties of the nanostructures' shape significantly influence the electrochemical NO3RR by enhancing the kinetics of charge transfer. This study seeks to advance research on morphology‐dependent electrochemical NO3RR through the strategic control of local electric field intensity in electrocatalysts.
- Research Article
18
- 10.1002/adfm.202305254
- Jul 27, 2023
- Advanced Functional Materials
Abstract The high activity of nano‐sized metal particles (NMPs) makes it easy to appear uncontrolled aggregation, which seriously affects Li/Na storage in electrode materials. Introducing adaptive substrates with proper affinity to NMPs is an effective strategy that optimizes the stability and capacity of the related electrodes. Herein, a comprehensive strategy for the fabrication of adaptive interfacial contacts between metallic Cu nanoparticles (NPs) and triphenyl‐substituted triazine graphdiyne (TPTG) substrates is reported. The sp C in the acetylenic linkers and N heteroatoms in the triazine groups synergistically stabilized the Cu NPs loaded onto the TPTG substrates. The stabilizing effect of the TPTG substrate induces a reversible lattice change of the Cu NPs during the charge–discharge process, thus efficiently facilitating the stable transfer of Li+/Na+. Intrinsic mechanism analysis indicates that the heterojunction contact interface of Cu NPs/TPTG provides branched charge transfer pathways from Li/Na to the Cu NPs and TPTG substrates, which synergistically adjusts the affinity to Li/Na atoms and ultimately improves the electrochemical performance in Li/Na storage. The investigation of the structure–property relationship deepens the understanding of the function of heterointerfaces, which is essential for optimizing the performance of energy storage devices.
- Research Article
4
- 10.1002/anie.202316936
- Jan 18, 2024
- Angewandte Chemie International Edition
Copper is a crucial catalyst in the synthesis of graphdiyne (GDY). However, as catalysts, the final fate of the copper ions has hardly been concerned, which are usually treated as impurities. Here, it is observed that after simple washing with water and ethanol, GDY still contains a certain amount of copper ions, and demonstrated that the copper ions are adsorbed at the atomic layers of GDY. Furthermore, we transformed in situ the copper ions into ultrathin Cu nanocrystals, and the obtained Cu/GDY hybrids can be generally converted into a series of metal/GDY hybrid materials, such as Ag/GDY, Au/GDY, Pt/GDY, Pd/GDY, and Rh/GDY. The Cu/GDY hybrids exhibit extraordinary surface enhanced Raman scattering effect and can be applied in pollutant efficient enrichment and detection.
- Research Article
9
- 10.1016/j.jallcom.2024.173757
- Feb 3, 2024
- Journal of Alloys and Compounds
In-situ XPS reveals the interfacial engineering of Co/Ce-BDC with graphdiyne (CnH2n-2) for effective photocatalytic H2 evolution
- Research Article
40
- 10.1002/anie.202216397
- Jan 10, 2023
- Angewandte Chemie International Edition
Vacancies can significantly affect the performance of metal oxide materials. Here, a gradient graphdiyne (GDY) induced Cu/O-dual-vacancies abundant Cu0.95 V2 O5 @GDY heterostructure material has been prepared as a competitive fast-charging anode material. Cu0.95 V2 O5 self-catalyzes the growth of gradient GDY with rich alkyne-alkene complex in the inner layer and rich alkyne bonds in the outer layer, leading to the formation of Cu and O vacancies in Cu0.95 V2 O5 . The synergistic effect of vacancies and gradient GDY results in the electron redistribution at the hetero-interface to drive the generation of a built-in electric field. Thus, the Li-ion transport kinetics, electrochemical reaction reversibility and Li storage sites of Cu0.95 V2 O5 are greatly enhanced. The Cu0.95 V2 O5 @GDY anodes show excellent fast-charging performance with high capacities and negligible capacity decay for 10 000 cycles and 20 000 cycles at extremely high current densities of 5 A g-1 and 10 A g-1 , respectively. Over 30 % of capacity can be delivered in 35 seconds.
- Research Article
15
- 10.1073/pnas.2319525121
- Apr 2, 2024
- Proceedings of the National Academy of Sciences of the United States of America
The fine regulation of catalysts by the atomic-level removal of inactive atoms can promote the active site exposure for performance enhancement, whereas suffering from the difficulty in controllably removing atoms using current micro/nano-scale material fabrication technologies. Here, we developed a surface atom knockout method to promote the active site exposure in an alloy catalyst. Taking Cu3Pd alloy as an example, it refers to assemble a battery using Cu3Pd and Zn as cathode and anode, the charge process of which proceeds at about 1.1 V, equal to the theoretical potential difference between Cu2+/Cu and Zn2+/Zn, suggesting the electricity-driven dissolution of Cu atoms. The precise knockout of Cu atoms is confirmed by the linear relationship between the amount of the removed Cu atoms and the battery cumulative specific capacity, which is attributed to the inherent atom-electron-capacity correspondence. We observed the surface atom knockout process at different stages and studied the evolution of the chemical environment. The alloy catalyst achieves a higher current density for oxygen reduction reaction compared to the original alloy and Pt/C. This work provides an atomic fabrication method for material synthesis and regulation toward the wide applications in catalysis, energy, and others.
- Research Article
5
- 10.1039/d3sc01393f
- Jan 1, 2023
- Chemical Science
Graphdiyne (GDY) is a promising material possessing extensive electronic tunability, high π conjugacy, and ordered porosity at a molecular level for the sp/sp2-hybridized periodic structures. Despite these advantages, the preparation of soluble and crystalline graphdiyne is limited by the relatively compact stacking interactions, mostly existing in thick-layer and insoluble solids. Herein, we proposed a strategy of "framework charge-induced intercalation (FCII)" for the synthesis of a soluble (4.3 mg ml-1) and yet interlayer-expanded (∼0.6 Å) crystalline ionic graphdiyne, named as N+-GDY, through regulating the interlayer interactions. The skeleton of such a sample is positively charged, and then the negative ions migrate to the interlayer to expand the space, endowing the N+-GDY with solution processability. The crystal structure of N+-GDY is proved through analysis of HR-TEM images under different axes of observation and theoretical simulations. The resulting N+-GDY possesses high dispersity in organic solvents to produce a pure-solution phase which is conducive to the formation of oriented N+-GDY films, accompanied by exfoliation-nanosheet restacking. The film exhibits a conductivity of 0.014 S m-1, enabling its applications in electronic devices.
- Research Article
33
- 10.1016/j.electacta.2022.140071
- Feb 15, 2022
- Electrochimica Acta
Hierarchical 3D flower like cobalt hydroxide as an efficient bifunctional electrocatalyst for water splitting
- Research Article
20
- 10.31635/renewables.022.202200002
- Jan 20, 2023
- Renewables
Thin Films Fabricated by Pulsed Laser Deposition for Electrocatalysis
- Research Article
13
- 10.1007/s40242-019-8344-x
- Mar 13, 2019
- Chemical Research in Chinese Universities
We used the one-step hydrothermal controlled synthesis method for Co-Ni3S2 ultrathin nanosheets grown directly on nickel foam(NF). The as-synthesized Co-Ni3S2/NF showed enhanced activities in the hydrogen evolution reaction(HER), oxygen evolution reaction(OER) and better overall water splitting(OWS) efficiency than the un-doped Ni3S2/NF. The voltage of Co-Ni3S2/NF for OWS was only 1.58 V at the current density of 10 mA/cm2 and with long time(>30 h) current output during the current-density(i-t) test. The good i-t performance was also observed in both HER and OER processes. Additionally, the Co-Ni3S2/NF showed a large current density(>1 A/cm2) for both HER and OER. When the current densities reached 100 and 1000 mA/cm2, the required overpotentials for Co-Ni3S2/NF were 0.35 and 0.75 V for OER and 0.30 and 0.85 V for HER. Therefore, after introducing Co, th e activity of Ni3S2-based material was strongly enhanced.
- Research Article
27
- 10.31635/ccschem.021.202100991
- Aug 11, 2021
- CCS Chemistry
Magnetocatalysis: The Interplay between the Magnetic Field and Electrocatalysis
- Research Article
61
- 10.1016/j.ijhydene.2020.07.194
- Aug 11, 2020
- International Journal of Hydrogen Energy
Novel 13X Zeolite/PANI electrocatalyst for hydrogen and oxygen evolution reaction
- Research Article
16
- 10.1016/j.ijhydene.2023.01.212
- Feb 6, 2023
- International Journal of Hydrogen Energy
Constructing microstructures in nickel-iron layered double hydroxide electrocatalysts by cobalt doping for efficient overall water splitting
- Research Article
27
- 10.1016/j.cej.2023.142592
- Mar 24, 2023
- Chemical Engineering Journal
In-situ construction of hexagonal-star-shaped MnCo2S4@MoS2 boosting overall water splitting performance at large-current-density: Compositional-electronic regulation, functions, and mechanisms
- Research Article
49
- 10.1016/j.apcatb.2022.121151
- Jan 31, 2022
- Applied Catalysis B: Environmental
Functional group scission-induced lattice strain in chiral macromolecular metal-organic framework arrays for electrocatalytic overall water splitting
- Research Article
55
- 10.31635/ccschem.022.202201796
- Apr 22, 2022
- CCS Chemistry
Computational Prediction of Graphdiyne-Supported Three-Atom Single-Cluster Catalysts
- Research Article
- 10.1021/acsami.5c01834
- May 7, 2025
- ACS applied materials & interfaces
Developing heterostructures with high electrical conductivity and appropriate adsorption strength for oxygen intermediates is a crucial strategy to reduce the energy consumption of overall water splitting (OWS) and enhance the economic viability of hydrogen energy. This article proposes a novel metallic heterostructure (NiCoP@Co3S4) that is in situ grown on nickel foam. The composite of NiCoP and Co3S4 not only promotes effective charge transfer in the heterojunction and accelerates the kinetics of the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) but also optimizes the electronic structure of the catalyst through interface engineering. Density functional theory (DFT) calculations demonstrate that the formation of the heterostructure significantly increases the density of electronic states near the Fermi level (EF), thereby enhancing conductivity. Moreover, the d-band center of NiCoP@Co3S4 shifts closer to EF, which enhances the binding strength of reaction intermediates to the catalyst's active sites. This shift lowers the reaction activation energy and thus promotes the catalytic process. Experimental results show that the NiCoP@Co3S4 heterostructure exhibits excellent performance in both HER (η10 = 62 mV) and OER (η10 = 203 mV). An electrolyzer composed of NiCoP@Co3S4 electrodes requires only a potential of 1.48 V to achieve a current density of 10 mA cm-2. Additionally, it demonstrates good stability over 100 h of testing, outperforming the Pt/C || RuO2 catalyst (1.51 V@10 mA cm-2). This work provides an effective approach to achieving efficient water splitting for hydrogen production at low overpotentials through the self-regulation of charge in heterostructures, offering new insights for the design of efficient non-noble metal-based electrocatalysts.
- Research Article
- 10.1002/smll.202504837
- Jun 16, 2025
- Small (Weinheim an Der Bergstrasse, Germany)
Efficient hydrogen (H2) generation from electrochemical overall water splitting (OWS) is key to a sustainable H2 economy. Low‐cost transition metal‐based catalysts, such as Ni‐ and Co‐based phosphides, have gained attention for the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) due to their excellent corrosion resistance and high electrical conductivity. In particular, bimetallic Ni and Co‐based phosphide catalysts are considered highly efficient electrocatalysts for OWS due to their abundant adsorption sites and low adsorption energy for hydrogen species. However, improving their stability and activity remains challenging. Herein, a Ce doping NiCo phosphide catalyst is presented with vary Ce amount (Cex‐NiCoP) supported on nickel foam (NF) with multi‐site functionality, achieving highly efficient HER performance comparable to benchmark platinum catalysts support carbon fiber or NF (Pt/C or Pt/NF). Comprehensive characterization results show that the optimal amount of Ce doping significantly influences the electronic structure of the catalyst, preventing the formation of Ni5P4 and CeO2, promoting the dominant NiCoP phase. This modification enhances the catalyst's hydrophilicity, improving the HER activity significantly. Remarkably, the catalyst also demonstrates exceptional OER performance, making it a highly active and stable bifunctional catalyst for OWS, with the highest energy efficiency of 96.7%.
- Research Article
113
- 10.1007/s12274-020-3006-3
- Aug 15, 2020
- Nano Research
Efficient and robust noble-metal-free bifunctional electrocatalysts for overall water splitting (OWS) is of great importance to realize the large-scale hydrogen production. Herein, we report the growth of undoped and Cr-doped NiCo2O4 (Cr-NiCo2O4) nanoneedles (NNs) on nickel foam (NF) as bifunctional electrocatalysts for both hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). We demonstrate that Cr-doping significantly improves activity for HER and OER by increasing the conductivity of NNs and allowing more active sites on NNs electrochemically accessible. When amorphous FeOOH is electrodeposited on the surface of Cr-NiCo2O4 NNs, the resulting FeOOH/Cr-NiCo2O4/NF exhibits itself as an excellent bifunctional catalyst for OWS. In the two-electrode cell where FeOOH/Cr-NiCo2O4/NF is used both as cathode and anode for OWS, a cell voltage of only 1.65 V is required to achieve an electrolysis current density of 100 mA·cm−2. In addition, the catalyst shows a very high stability for OWS, the two-electrode cell can operate at a consist current density of 20 mA·cm−2 for 10 h OWS with the cell voltage being stable at ca. 1.60 V. These results demonstrate that FeOOH/Cr-NiCo2O4/NF possesses an OWS performance superior to most of transition-metal based bifunctional electrocatalysts working in alkaline medium. The excellent bifunctional activity and stability of FeOOH/Cr-NiCo2O4/NF are attributed to the following reasons: (i) The NN structure provides a large specific surface area; (ii) the high conductivity of Cr-NiCo2O4 enables more active centers on the far-end part of NNs to be electrochemically reached; (iii) the deposition of FeOOH supplies additional active sites for OWS.
- Research Article
13
- 10.1016/j.jcis.2024.07.019
- Jul 4, 2024
- Journal of Colloid And Interface Science
Electronic transfer and structural reconstruction in porous NF/FeNiP-CoP@NC heterostructure for robust overall water splitting in alkaline electrolytes
- Research Article
48
- 10.1016/j.ijhydene.2020.11.271
- Jan 7, 2021
- International Journal of Hydrogen Energy
Thin-film iron-oxide nanobeads as bifunctional electrocatalyst for high activity overall water splitting
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9
- 10.1016/j.ijhydene.2023.09.309
- Oct 25, 2023
- International Journal of Hydrogen Energy
Nanorods of nitrogen-rich copper MOF in high-performance bifunctional electrocatalysis for oxygen and hydrogen evolution reactions
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