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International Journal of Electrochemical Science · 2023 · IF 1.5

Nanocavity-enriched Porous Cu2O Catalyst for Selective CO2 Reduction to Multicarbon Products through the Nanoconfinement Effect

Haiyu Wang,Yan Huang,Huamin Li,Haibin Wang,Kaili Yao,Tan Jing,Songhua Chen,Lihua Liu,Hongyan Liang

Incorporating a nanoporous surface and a nanocavity into an electrocatalytic platform increases the active surface area and local mass density. Construct of specialized geometrical structures that are protected from harsh electrochemical environments is critical, albeit challenging, for improving the catalytic performance of CO 2 reduction (CO 2 R). In this study, we successfully incorporate porosity and a cavity into a single structure, a porous copper nanocavity, derived from a pristine porous Cu 2 O template. We compare the CO 2 R catalytic performance of the porous copper nanocavity with that of a bulky catalyst derived from commercial Cu 2 O, and the former shows superior selectivity for multicarbon products. Operando Raman spectra suggest that the enhanced CO 2 R catalytic performance results from high *CO coverage and the confinement of intermediates in the porous copper nanocavity. These results may pave the way for the rational geometric design of selective catalysts for CO 2 R.

研究领域: 材料科学 · 电化学
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Journal of Materials Chemistry A · 2018 ·Vol. 7 ·期 9 ·4469-4479 · IF 9.931

Cellular carbon-wrapped FeSe2 nanocavities with ultrathin walls and multiple rooms for ion diffusion-confined ultrafast sodium storage

Yongchao Tang,Zongbin Zhao,Xiaojuan Hao,Yue Wei,Han Zhang,Yanfeng Dong,Yuwei Wang,Xin Pan,Yanan Hou,Xuzhen Wang,Jieshan Qiu

Sodium-ion batteries (SIBs) with high energy/power density have been in urgent demand for various power applications. Upgrading the electrochemical dynamics of electrode materials is crucial to achieve this goal. Herein, we exhibit delicately synthesized cellular carbon-wrapped FeSe2 nanocavities (h-FeSe2@PC) with sub-5 nm ultrathin walls and multiple rooms for ultrafast sodium storage. Unlike with the conventional interphase Kirkendall effect, the multi-room FeSe2 nanocavities were formed via an exotic stress-induced cracking–hollowing reassembly mechanism. Benefiting from their unique multi-hierarchy, more than 93% pseudocapacitive capacity contribution was recognized in an h-FeSe2@PC anode, featuring ultrafast dynamics. As a result, h-FeSe2@PC displayed an extremely low-decay (9.5%) rate capability, ultrastable cyclability (over 2000 loops with 98.5% capacity retention), and high energy/power densities (670.7 W h kg−1/35.3 kW kg−1 at 20 A g−1). The results of multiple analyses and comparisons showed that the dynamics-promoted superior performance was correlated almost completely to the applied FeSe2 in h-FeSe2@PC by shortening the Na+-diffusion length to near the accessible limit (<10 nm) and to the fast electron transfer ensured by the cellular carbon. The exhibited dynamics-oriented materials design could open up an avenue to aid the further development of high-performance electrodes.

研究领域: 材料科学 · 电化学
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RARE METALS · 2024 ·Vol. 43 ·期 4 ·1513-1523 · IF 9.6

Nanocavity enriched CuPd alloy with high selectivity for CO2 electroreduction toward C2H4

Zhang Ze-Yu,Wang Hai-Bin,Zhang Fei-Fei,Li Jing-Wei,Hu Xin-Zhuo,Yan Si-Wei,Bai Yi-Ming,Zhang Xun,Shen Gu-Rong,Yin Peng-Fei,Yang Jing,Dong Cun-Ku,Mao Jing,Liu Hui,Du Xi-Wen

Electrocatalysis of CO 2 reduction reaction is an effective way to convert CO 2 into high value-added products, but the selectivity of Cu-based catalysts for C 2+ products needs to be improved due to the high energy barrier of C–C coupling. Therefore, a viable catalyst design strategy to decrease energy barrier of C–C coupling should be put forward. Here, a nanocavity-enriched CuPd single atom alloy (CuPd SAA) catalyst is designed to promote C–C coupling process. The faradaic efficiency of CuPd SAA for ethylene and C 2+ reaches 75.6% and 85.7% at − 0.7 V versus reversible hydrogen electrode (RHE), respectively. Based on the results given by in situ characterization, the porous hollow structure dramatically increases the ratio of the linear-bond *CO, thus enhancing the faradaic efficiency for ethylene. Density functional theory (DFT) calculation reveals that the Pd doping can regulate the electronic structure of neighboring Cu atoms to decrease the energy barrier of C–C coupling, further improving the faradaic efficiency. This work provides a new idea for designing catalyst with high selectivity for ethylene. Graphical abstract

研究领域: 材料科学 · 化学 · 电化学 · 催化
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ANALYST · 2024 · IF 3.6

Mesothelin microsensor based on embedded thionine electronic media within imprinted polymer on acupuncture needle electrode

Yi Zhang,Xue Kong,Haiyang Guo,Jing Wang,Zheng-Zhi Yin

An electrochemical microsensor for mesothelin (MSLN) based on an acupuncture needle (AN) was constructed in this work. To prepare the microsensor, MSLN was self-assembled on 4-mercaptophenylboric acid (4-MPBA) by an interaction force between the external cis-diol and phenylboronic acid. This was followed by the gradual electropolymerization of thionine (TH) and eriochrome black T (EBT) around the anchored protein. The thickness of the surface imprinted layers influenced the sensing performance and needed to be smaller than the height of the anchored protein. The polymerized EBT was not electrically active, but the polymerized TH provided a significant electrochemical signal. Therefore, electron transfer smoothly proceeded through the eluted nanocavities. The imprinted nanocavities were highly selective toward MSLN, and the rebinding of insulating proteins reduced the electrochemical signal of the embedded pTH. The functionalized interface was characterized by SEM and electrochemical methods, and the preparation conditions were studied. After optimization, the sensor showed a linear response in the range of 0.1 to 1000 ng/mL with a detection limit of 10 pg/mL, indicating good performance compared with other reported methods. This microsensor also showed high specificity and stability, which can be attributed to the fine complementation of the imprinted organic nanocavities. The sensitivity of this sensor was related to the nanocavities used for electron transport around the AuNPs. In the future, microsensors that can directly provide electrochemical signals are expected to play important roles especially on AN matrices.

研究领域: 生物化学 · 电化学 · 传感器 · 纳米技术 · 医疗器械
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