CHINESE JOURNAL OF CATALYSIS
·
2023
·
IF 16.5
Na Zhou,Jiazhi Wang,Ning Zhang,Zhi Wang,Hengguo Wang,Gang Huang,Di Bao,Haixia Zhong,Xinbo Zhang
Electrochemical conversion of nitrate (NO 3 − ) pollutants into chemical feedstock and fuel ammonia (NH 3 ) can contribute to sustainable mitigation of the current severe energy and environmental crises. However, the electrocatalytic NO 3 − reduction to NH 3 (NRA) involves a sluggish multielectron and proton transfer process that competes with the hydrogen evolution reaction (HER) in aqueous media, imposing great challenges in developing highly selective catalysts for NRA. In this study, we developed a copper and copper-tetracyanoquinodimethane composite catalyst (Cu@CuTCNQ), which possesses a high density of copper vacancy defects. This catalyst has been proven to be efficient for NRA through an in situ electrochemical reconstruction method. The structural evolution of CuTCNQ during NRA was investigated by in situ Raman spectroscopy, which indicated an accelerated charge transfer from the CuTCNQ substrate to the derived Cu, which facilitated the adsorption activation of NO 3 − . The obtained Cu@CuTCNQ exhibited an excellent catalytic performance for NRA, with a Faradaic efficiency of 96.4% and productivity of 144.8 μmol h −1 cm −2 at −0.6 V vs . a reversible hydrogen electrode, superior to Cu nanoparticle counterparts and most Cu-based catalysts. Cu vacancy defects and sufficient interfacial charge transfer synergistically optimize the charge distribution of Cu active sites, reduce the energy barrier for NO 3 − adsorption, and promote deoxidation and hydrogenation processes, thus enhancing NRA and selectivity.
研究领域:
材料科学
·
环境科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF POWER SOURCES
·
2024
·
IF 8.1
Tao-Long Wu,Peng-Fei Qiu,Xiu-Niang Tan,Manlin Chen,Chenchen Wang,Yan Zhou,Zai-Yin Huang
Hierarchical core-shell hetero-arrays with well-controlled morphology, rational combination of hybrid electrochemical active materials are regarded as promising candidate electrodes for supercapacitors due to their excellent redox activity and electrical conductivity. However, their inferior rate performance and poor long-term cycling stability hinder their practical applications and still of great challenge. In this work, three hierarchical core-shell CuTCNQ@MWO 4 /CF ( TCNQ = 7,7,8,8-Tetracyanoquinonedimethane; M = Cu, Co and Ni ) hetero-arrays on Cu foam with different morphology are successfully constructed by in situ conductive metal-organic framework templated synthetic route of an inter-facial growth and a hydrothermal synthesis process. The crystallinity of MWO 4 decorated on the conductive CuTCNQ nanoarrays plays important role in their electrochemical performances. Especially, the hierarchical tree-like CuTCNQ@CuWO 4 /CF hetero-arrays electrode can be used as high-performance positive electrode materials for supercapacitor, which exhibits excellent electrochemical properties with a high area capacitance (1073.3 mF/cm 2 at 1 mA/cm 2 ), excellent rate capability, low resistances and outstanding cycling stability with capacitance retention of 88.6% at 30 mA/cm 2 after 10000 cycles. What's more, the CuTCNQ@CuWO 4 //AC ASC device delivers a high energy density of 0.075 mW h/cm 2 (45 W h/kg) at a power density of 0.8 mW/cm 2 (480 W/kg) and still achieves a energy density of 0.053 mW h/cm 2 (32.1 W h/kg) at a power density of 4.00 mW/cm 2 (2424 W/kg). Thus, this work demonstrates that a rational and effective strategy is explored to prepare hierarchical hetero-arrays with different morphology from conductive MOF-templated for high-performance energy storage in practical application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Applied Materials & Interfaces
·
2022
·
IF 10.383
Zhi Jiang,Hezhuang Liu,Jihua Zou,Yixuan Huang,Zhaoquan Xu,Caihong Li,Desheng Liu
With the rapid advances in metal halide perovskite optoelectronics, eliminating toxic lead from perovskites has been an urgent demand. However, state-of-the-art lead-free perovskite photodetectors are still challenged with issues of low photoresponse, poor stability, etc. Here, all-inorganic lead-free perovskite (Cs3Cu2I5) single crystals that possess good stability under air exposure are synthesized via a facile solid reaction method. Meanwhile, a higher photoluminescence quantum yield of 95.2% and a prolonged carrier lifetime of 1.127 μs are obtained by further optimizing the synthesis. Benefiting from the polyporous surface and hollow structure of Cu-7,7,8,8-tetracyanoquinodimethane (CuTCNQ) microtubes, more Cs3Cu2I5 nanocrystals can adhere on the innershell and outershell of CuTCNQ-15 microtubes. This unique structure contributes to the improved efficiency of utilizing incident light and promotes charge carrier generation and transportation. As a result, the hierarchical CuTCNQ/Cs3Cu2I5 (hollow microtube/nanocrystal) heterostructure phototransistor exhibits a high responsivity of 88.36 A W–1 and a large detectivity of 1.66 × 1012Jones. The proposed lead-free perovskites and mixed-dimensional heterojunctions are promising for sensitive light detection.
研究领域:
材料科学
·
光学工程
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2023
·
IF 3.3
Qijiu Deng,Zhiyun Zhao,Lei Mao,Yiming Zou,Bo Gou,Yinling Yan,Weihua Zhang,Rong Yang,Yunhua Xu
The seriously dissolution of the intermediate into the organic electrolyte has been the key limitation for metal-organic compounds in K-ion batteries. Here, we initially inhibit the dissolution of intermediate products (TCNQ 0 ) with a highly conducting polymer (polypyrrole, PPy) coated on the CuTCNQ. And the adsorption energy between the conductive polymer PPy and the intermediate product TCNQ can be significantly enhanced (−0.55 eV) as compared to the TCNQ molecules (0.21 eV), which can restrain the free intermediate product dissolved in the organic electrolyte, resulting in an enhanced cyclic stability as well as rate performance. Additionally, the highly conductive PPy exhibits flexible structure, which can weaken the interface effect between the electrode and the coating layer. This work provides further understanding on surface coating on metal-organic compounds and has significant basic scientific sense for the in-depth research of K-ion batteries.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）