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Jian Li;Roberto Valenza;Sophia Haussener; 《Small (Weinheim an der Bergstrasse, Germany)》2024,20(33):2310467
Electroreduction of nitrate to ammonia provides an interesting pathway for wastewater treatment and valorization. Cu-based catalysts are active for the conversion of NO3− to NO2− but suffer from an inefficient hydrogenation process of NO2−. Herein, CuxO/N-doped graphdiyne (CuxO/N-GDY) with pyridine N configuration are in situ prepared in one pot. Benefiting from the synergistic effect of pyridinic N in GDY and CuxO, the prepared CuxO/N-GDY tested in a commercial H-cell achieved a faradaic efficiency of 85% toward NH3 at -0.5 V versus RHE with a production rate of 340 µmol h−1 mgcat−1 in 0.1 M KNO3. When integrating the CuxO/N-GDY in an anion exchange membrane flow electrolyzer, a maximum Faradaic efficiency of 89% is achieved at a voltage of 2.3 V and the production rate is 1680 µmol h−1 mgcat−1 at 3.3 V in 0.1 M KNO3 at room temperature. Operation at 40 °C further promoted the overall reaction kinetics of NO3− to NH3, but penalized its selectivity with respect to hydrogen evolution reaction. The high selectivity and production rate in this device configuration demonstrate its potential for industrial application. 相似文献
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Huidi Yu Yurui Xue Lan Hui Chao Zhang Yingjie Zhao Zhibo Li Yuliang Li 《Advanced functional materials》2018,28(19)
The first utilization of nitrogen‐doped graphdiyne (NGDY) as an efficient catalytic promoter for hydrogen evolution reaction (HER) is reported. X‐ray powder diffraction and X‐ray photoelectron spectroscopy studies indicate the presence of strong interactions between NGDY and MoS2, which should effectively facilitate the charge transport behavior and improvement of the HER kinetics. The creative hybridization of MoS2 and NGDY endows such heterostructure with structural and compositional advantages for boosting the catalytic activity (low overpotential of 186 mV at 10 mA cm?2 and Tafel slope of 63 mV dec?1) and extraordinary stability (higher than all reported MoS2‐based materials and even better than that of commercial Pt and almost all benchmarked electrocatalysts). All of the results not only demonstrate that NGDY can be used as an effective catalytic promoter for hydrogen production, but also provide new strategy for fabricating efficient water‐splitting electrodes. 相似文献
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Jianjiang He Tiantian Lu Kun Wang Xin Wang Xiaodong Li Xiangyan Shen Juan Gao Wenyan Si Ze Yang Changshui Huang 《Advanced functional materials》2021,31(5):2005933
Developing new electrode materials with a regular channel for stable storage and diffusion of potassium (K) ions is crucial to alleviating the ubiquitous problems in K-ion batteries (KIBs) such as slow diffusion rate, huge volume expansion, and unstable interface by the large K ion radius. Herein, electrode material with a facile diffusion pathway, vast space for volume expansion, and good interfacial compatibility are found to be necessary. Fluoride graphdiyne (F-GDY) is illustrated for its expanded conductive skeleton, uniform structural pores, and well-distributed F atoms. First-principles computations and electrochemical characterizations reveal the high reversible capacity and cyclic stability for the instanced F-GDY electrode through the ultralow diffusion barrier, abundant exposed active sites, and stable KF-enriched solid electrolyte interphase film. The F-GDY anode exhibits a capacity of 320 mAh g−1 at 50 mA g−1, and 120 mAh g−1 at 1000 mA g−1 for 1800 cycles. These electrochemical performances of F-GDY anode are superior than those of many other carbon materials reported to date, providing us with a new insight into the design of an electrode for KIBs. 相似文献
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The successful synthesis of stacking graphdiynes has stimulated numerous fascinating applications. However, it still remains challenging to prepare atomically precise 2D graphdiyne and other graphyne‐based structures. The development of on‐surface synthesis has contributed to many secondary graphyne‐based structures that are directive in fabricating extended graphyne networks. Herein, the recent progress concerning on‐surface synthesis of graphyne‐based nanostructures, especially atomically precise graphdiyne nanowires, is summarized. 相似文献
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Huimin Liu;Lu Qi;Zhaoyang Chen;Shuya Zhao;Xiaoyu Luan;Jiayu Yan;Zhiqiang Zheng;Fanle Bu;Yurui Xue;Yuliang Li; 《Small (Weinheim an der Bergstrasse, Germany)》2024,20(37):2401347
A challenge facing the chlor-alkali process is the lack of electrocatalyst with high activity and selectivity for the efficient industrial production of chlorine. Herein the authors report a new electrocatalyst that can generate multi-interface structure by in situ growth of graphdiyne on the surface of cobalt oxides (GDY/Co3O4), which shows great potential in highly selective and efficient chlorine production. This result is due to the strong electron transfer and high density charge transport between GDY and Co3O4 and the interconversion of the mixed valence states of the Co atoms itself. These intrinsic characteristics efficiently enhance the conductivity of the catalyst, facilitate the reaction kinetics, and improve the overall catalytic selectivity and activity. Besides, the protective effect of the formed GDY layer is remarkable endowing the catalyst with excellent stability. The catalyst can selectively produce chlorine in low-concentration of NaCl aqueous solution at room temperature and pressure with the highest Faraday efficiency of 80.67% and an active chlorine yield rate of 184.40 mg h−1 cm−2, as well as superior long-term stability. 相似文献
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Fulai Liu Xutao Gao Rui Shi Jinfan Xiong Zhengxiao Guo Edmund C. M. Tse Yong Chen 《Advanced functional materials》2024,34(6):2310274
Adipic acid (AA) is a crucial feedstock for nylon polymers, and is industrially produced by thermal oxidation of cyclohexanone/cyclohexanol mixture (KA oil). However, this process consumes large quantities of corrosive nitric acid as oxidants, while emits ozone-depleting greenhouse gas N2O. Here, an electrocatalytic strategy for selective oxidation of KA oil to AA coupled with H2 evolution over a Co3O4/graphdiyne cooperative catalyst (Co3O4/GDY) is reported. The Co3O4/GDY displays high electrooxidation activity of KA oil to AA (100 mA cm−2 at ≈1.5 V vs RHE), outperforming all the reported findings. Detailed ex situ and in situ experimental studies, theoretical calculations, and molecular dynamic simulations reveal that GDY not only facilitates the enrichment of cyclohexanone on the catalyst surface in aqueous medium, but also upshifts the d-band center of Co sites, strengthening the adsorption/activation of cyclohexanone. This study offers a green route for AA synthesis and proposes a GDY interface engineering strategy for efficient electrooxidation. 相似文献
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Jing Xu;Qian Li;Yan Shang;Zhenlu Liu;Zhiliang Jin; 《Solar RRL》2024,8(4):2301006
Inhibiting the recombination of photoexcited hole–electron pairs is the crucial for efficient hydrogen-producing by photocatalytic water splitting under visible light. Although Ag2Mo2O7 has excellent photoelectrochemical properties and strong morphological plasticity, its hydrogen-producing activity is inhibited due to its low separation efficiency of photogenerated carriers and small photoresponse range. Therefore, graphdiyne (GDY) is prepared using alkynyl anions and compounded with Ag2Mo2O7 by electrostatic self-assembly. The hydrogen-producing capacity of the composite catalyst GDY/Ag2Mo2O7 reaches up to 8156.6 μmol g−1 h−1, what is more, the photocatalytic hydrogen-producing capacity of Ag2Mo2O7, GDY, and GDY/Ag2Mo2O7 is investigated by in situ X-ray photoelectron spectroscopy, electrochemical testing, fluorescence analysis, and density functional theory calculation. The consequences display that the composite catalyst GDY/Ag2Mo2O7 shows the best fluorescence quenching effect and the highest photocurrent response intensity. In the final analysis, the preeminent photocatalytic hydrogen-producing performance of the composition GDY/Ag2Mo2O7 is due to the establishment of type S heterojunction, and the migration rate of photogenerated electrons is increased and the migration path is shortened. This contributes a practical tactics to effectively enhance the capacity of photocatalytic hydrogen-producing by solving the problem of serious recombination of photogenerated carriers. 相似文献
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