Small Structures
·
2023
·Vol. 4
·期 11
·2300177
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IF 15.9
Yi-lei Li,Qing Zhao,Xu-jia Liu,Ying Liu,Ying-juan Hao,Xiao-jing Wang,Xin-ying Liu,Diane Hildebrandt,Feng-yu Li,Fa-tang Li
Precise regulation of photogenic electron transfer path plays an important role in improving photocatalytic carbon dioxide reduction efficiency and product selectivity. Herein, under the guidance of density functional theory calculation, the interface chemical bond (Co N 2 bond) at the atomic level is designed, and g-C 3 N 4 /CoCo-layered double hydroxide (LDH) heterostructure is manufactured. CoCo-LDH with water oxidation ability and g-C 3 N 4 were combined to construct S-scheme heterojunction with redox ability. The valence band and conduction band of g-C 3 N 4 and CoCo-LDH are precisely connected by the interfacial Co N 2 bond, which realizes the high-speed transfer of electron transport. Despite the absence of cocatalyst, the heterojunction exhibits high water oxidation and carbon reduction capacity due to the precise regulation of Co N 2 bonds. Theoretical calculations and experimental results show that the addition of CoCo-LDH: reduces the oxidation overpotential of water to provide more H protons; regulates the delocalization charge of g-C 3 N 4 ; and reduces the energy barrier of the CO 2 intermediate (*COOH) in the reduction half-reaction. The results show that the selectivity of carbon-based substances in the products was 100%, and the optimal CO yield was 71.39 μmol g −1 h −1 , which is among the highest values of g-C 3 N 4 -based photocatalysts.
研究领域:
材料科学
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环境科学
·
化学
✓ 已验证
产品关联
DOI
高影响因子
Nanoscale
·
2017
·Vol. 9
·期 42
·16256-16263
·
IF 7.367
Yuzhu Xue,Zhiyu Ren,Ying Xie,Shichao Du,Jun Wu,Huiyuan Meng,Honggang Fu
Manipulating the electrical conductivity and morphology of Co-based (hydr)oxides is significant for optimizing energy conversion in the oxygen evolution reaction (OER). Herein, 2D CoSex nanocrystalline-dotted porous CoCo layered double hydroxide nanosheets (Co–Se NSs) were designed and synthesized via a modified in situ reduction and interface-directed assembly in an inert atmosphere. During the synchronous reduction/precipitation reaction between Co2+-oleylamine and NaHSe at the toluene–water interface, the hydrated Co–O and Co–Se clusters are generated and sequentially assemble under strong extrusion driven by the interfacial tension. Owing to the enriched vacancies on the lateral surfaces, the obtained loose and porous Co–Se NS presents low crystallinity. Moreover, electrons could spontaneously transfer from the CoCo LDH to the neighboring CoSex nanocrystallites due to the stronger electron-withdrawing capability of metallic CoSex, and thus more Co atoms in the CoCo layered double hydroxide (LDH) present a high oxidation state. This synergistic manipulation in the structure, component, and electron configuration of the Co–Se NS can increase the density of the OER active-sites, improve the electrical conductivity, and also offer a large accessible surface area and permeable channels for ion adsorption and transport. As a result, the resulting Co–Se NSs feature high catalytic activity towards OER, in particular a low onset potential of 1.48 V and an overpotential of only 290 mV at a current density of 10 mA cm−2 for the Co-Se-2 NS, as well as good stability in an accelerated durability test. The strategy developed here provides a reliable and valid way to synthesize multicomponent NSs, and is able to be extended to other areas of application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
·
2022
·
IF 6.371
Yong Xie,Si-Jie Li,Jie-Ping Huang,Rui Qiu,Zhao-Qing Liu,Nan Li
Oxygen reaction plays a vital role in energy storage such as zinc-air battery and microbial fuel cell (MFC). Thus, it is necessary to search and develop non-precious metal electrocatalysts with remarkable activity. In this work, copper is cleverly doped into the octahedral sites of Co 9 S 8 to strengthen the Co Co bond and then combined with nitrogen-doped hollow carbon spheres to achieve high catalytic activity and durability for oxygen reduction reactions (ORR) and oxygen evolution reactions (OER). The prepared Cu-Co 9 S 8 -NHCS-1 exhibits the potential gap of 0.788 V between E j=10 of OER and E 1/2 of ORR. Moreover, the zinc-air battery with Cu-Co 9 S 8 -NHCS-1 cathode possesses a power density of 91.0 mW cm -2 and long-term stability over 120 h. The MFC using Cu-Co 9 S 8 -NHCS-1 cathode exhibits a power density of 924 ± 18 mW m -2 , higher than that of 862 ± 20 mW m -2 with Pt/C. These results indicate that the Cu-Co 9 S 8 -NHCS-1 is an excellent bifunctional electrocatalyst for ORR and OER, and has promising applications in energy conversion.
研究领域:
材料科学
·
电化学
·
能源转换与存储
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2022
·
IF 24.319
Jixiang Ji,Ruru Li,Hao Zhang,Yingnan Duan,Qian Liu,Haozhi Wang,Zhurui Shen
To date, the efficient photocatalytic conversion of CO 2 into high-value C2 products remains a great challenge. Herein, the Au-CeO 2 nanocomposite with Au-O-Ce sites at the micro-interface was developed to achieve a highly selective conversion of CO 2 into C 2 H 6 . This can be partially ascribed to the formation of key intermediates of COCO* was confirmed via in-situ Fourier transform infrared (FTIR) spectroscopy, indicating that the Au-CeO 2 micro-interface could prompt the multi-electron reduction of CO* before desorption, and enable the production of C2 species. Moreover, theoretical calculations suggested that Au-O-Ce sites at the micro-interface could reduce the energy barriers for the formation of COOH* and COCO*, facilitating the production of C 2 H 6 . Therefore, the Au-CeO 2 nanocomposite exhibited a C 2 H 6 production rate of 11.07 µmol g −1 h −1 and high electron selectivity of 93.1 % (product selectivity: 65.3 %), which is comparable with most state-of-the-art photocatalysts.
研究领域:
材料科学
·
环境科学
·
化学工程
·
催化
✓ 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）