In situ growth of Ni(x)Cu(1-x) alloy nanocatalysts on redox-reversible rutile (Nb,Ti)O₄ towards high-temperature carbon dioxide electrolysis.

In situ growth of Ni(x)Cu(1-x) alloy nanocatalysts on redox-reversible rutile (Nb,Ti)O₄ towards high-temperature carbon dioxide electrolysis.
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DOI:
10.1038/srep05156
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发表时间:
2014-06-03
期刊:
影响因子:
4.6
通讯作者:
Wu Y
Wu Y
中科院分区:
综合性期刊3区
文献类型:
--
作者:
Wei H;Xie K;Zhang J;Zhang Y;Wang Y;Qin Y;Cui J;Yan J;Wu Y

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本文报道了NixCu_(1-x)的原位生长(x = 0,0.25,0.50,0.75和1.0)合金化催化剂以锚和装饰氧化还原-可逆Nb1.33Ti0.67O4陶瓷基底,目的是通过在还原气氛中金属颗粒从陶瓷氧化物的晶格中直接出溶来定制复合材料的电催化活性在高温下。结合XRD、SEM、EDS、TGA、TEM和XPS分析证实了NixCu 1-x合金颗粒在氧化还原循环处理过程中完全可逆的出溶/溶解。TEM结果表明,合金颗粒以异质结的形式出溶并锚在高导电性Nb 1.33 Ti 0.67 O 4表面。系统研究了纳米NixCu 1-x/Nb1.33Ti0.67O4复合电极的电学性能,并将其与复合电极的电化学性能进行了关联。在高温还原气氛中,观察到改善的电极活性对合金成分的强烈依赖性。在固体氧化物电解槽中研究了NixCu 1-x/Nb1.33Ti0.67O4复合阴极直接电解CO2的性能。观察到的CO2裂解率与Ni组合物呈正相关;然而,Ni0.75Cu0.25结合了金属镍和铜的优点,因此使电流效率最大化。
In this paper, we report the in situ growth of NixCu1-x (x = 0, 0.25, 0.50, 0.75 and 1.0) alloy catalysts to anchor and decorate a redox-reversible Nb1.33Ti0.67O4 ceramic substrate with the aim of tailoring the electrocatalytic activity of the composite materials through direct exsolution of metal particles from the crystal lattice of a ceramic oxide in a reducing atmosphere at high temperatures. Combined analysis using XRD, SEM, EDS, TGA, TEM and XPS confirmed the completely reversible exsolution/dissolution of the NixCu1-x alloy particles during the redox cycling treatments. TEM results revealed that the alloy particles were exsolved to anchor onto the surface of highly electronically conducting Nb1.33Ti0.67O4 in the form of heterojunctions. The electrical properties of the nanosized NixCu1-x/Nb1.33Ti0.67O4 were systematically investigated and correlated to the electrochemical performance of the composite electrodes. A strong dependence of the improved electrode activity on the alloy compositions was observed in reducing atmospheres at high temperatures. Direct electrolysis of CO2 at the NixCu1-x/Nb1.33Ti0.67O4 composite cathodes was investigated in solid-oxide electrolysers. The CO2 splitting rates were observed to be positively correlated with the Ni composition; however, the Ni0.75Cu0.25 combined the advantages of metallic nickel and copper and therefore maximised the current efficiencies.
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