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Mesoporous Carbon Nanofibers Loaded with Ordered PtFe Alloy Nanoparticles for Electrocatalytic Nitrate Reduction to Ammonia
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作者 XIE Meng LUO Wei QIU Pengpeng 《Journal of Donghua University(English Edition)》 CAS 2024年第4期365-376,共12页
Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we... Highly dispersed bimetallic alloy nanoparticle electrocatalysts have been demonstrated to exhibit exceptional performance in driving the nitrate reduction reaction(NO_(3)RR)to generate ammonia(NH_(3)).In this study,we prepared mesoporous carbon nanofibers(mCNFs)functionalized with ordered PtFe alloys(O-PtFe-mCNFs)by a composite micelle interface-induced co-assembly method using poly(ethylene oxide)-block-polystyrene(PEO-b-PS)as a template.When employed as electrocatalysts,O-PtFe-mCNFs exhibited superior electrocatalytic performance for the NO_(3RR)compared to the mCNFs functionalized with disordered PtFe alloys(D-PtFe-mCNFs).Notably,the NH_(3)production performance was particularly outstanding,with a maximum NH_(3)yield of up to 959.6μmol/(h·cm~2).Furthermore,the Faraday efficiency(FE)was even 88.0%at-0.4 V vs.reversible hydrogen electrode(RHE).This finding provides compelling evidence of the potential of ordered PtFe alloy catalysts for the electrocatalytic NO_(3)RR. 展开更多
关键词 ordered PtFe alloy mesoporous carbon nanofiber(mCNF) nitrate reduction reaction(no3rr) ammonia(NH3)production reaction
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协同光电及热效应实现铜光阴极上等离激元催化高效硝酸根还原反应
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作者 陈振霖 薛静 +5 位作者 武磊 党昆 籍宏伟 陈春城 章宇超 赵进才 《Chinese Journal of Catalysis》 SCIE CAS CSCD 2024年第7期219-230,共12页
近年来,电催化硝酸根还原反应(NO_(3)RR)已经成为水处理和合成氨领域的研究热点.相比于传统的电催化剂,等离激元辅助的电催化反应通过将太阳能和电化学偏压同时施加到金属纳米结构上,在实现高效太阳能到化学能转化领域展现出了巨大潜力... 近年来,电催化硝酸根还原反应(NO_(3)RR)已经成为水处理和合成氨领域的研究热点.相比于传统的电催化剂,等离激元辅助的电催化反应通过将太阳能和电化学偏压同时施加到金属纳米结构上,在实现高效太阳能到化学能转化领域展现出了巨大潜力.然而,目前有关等离激元辅助NO_(3)RR的文献报道较少,已有的研究主要集中于利用金(Au)纳米结构的等离激元效应辅助增强NO_(3)RR.但Au对NO_(3)RR的本征电催化活性很差,这导致在等离激元辅助NO_(3)RR领域,氨的产率和法拉第效率难以令人满意.此外,对于等离激元辅助NO_(3)RR的机理研究不深入,例如如何区分等离激元产生的光电效应和光热效应对NO_(3)RR的影响,以及等离激元激发的金属纳米结构是如何影响NO_(3)RR过程等问题都尚未解决.因此,有必要采取有效的策略来深入探究等离激元辅助NO_(3)RR的内在机制,从而进一步提高其催化性能.铜(Cu)作为一种高效的硝酸根还原电催化剂,同时是一种典型的具有等离激元效应的金属材料.然而,目前关于利用Cu的等离激元效应辅助增强NO_(3)RR的报道很少.本文报道了利用Cu纳米线(CuNWs)的等离激元效应辅助增强NO_(3)RR性能.在等离激元激发条件下,CuNWs展现出较好的NO_(3)RR催化性能.在协同的光电和热效应的作用下,与暗态常温条件相比,催化性能提升了近2倍.经过400次循环伏安测试,CuNWs光阴极的电流密度仅下降到初始值的88%,而在黑暗条件下,CuNWs光阴极催化NO_(3)RR的电流密度则下降了43%.这表明光照同时显著提升了CuNWs催化NO_(3)RR的稳定性.产物分析结果表明,在-0.2到-0.4 V(相对于可逆氢电极)的宽电势范围内,CuNWs光阴极实现了接近100%的氨法拉第效率,并取得了较高的氨产率,超过了之前大多数报道的等离激元辅助Au催化剂的NO_(3)RR性能.通过活化能实验、微分电流实验以及升温实验,区分了等离激元激发产生的光电效应以及光热效应对NO_(3)RR的影响.通过原位拉曼光谱、在线差分电化学质谱以及原位电化学红外光谱技术,确定了CuNWs光阴极NO_(3)RR过程中的活性相及反应中间体.密度泛函理论计算结果表明,氨的脱附是NO_(3)RR的决速步.光生电子可以通过电子跃迁激发脱附机制促进氨的脱附从而抑制了氨在Cu表面的累积,弱化了氨对CuNWs光阴极的毒化作用.同时,光热效应也显著提升了NO_(3)RR的反应速率.因此,等离激元激发产生的光电和光热效应协同促进了NO_(3)RR性能,提高了CuNWs光阴极的活性与稳定性.将该策略拓展到其它Cu纳米材料上,同样展现出较好的等离激元促进效果.综上,本文提出了利用Cu的等离激元效应辅助增强电催化NO_(3)RR性能的策略,并验证了该策略在其它Cu纳米材料上的适用性.深入的机理研究揭示了同时耦合太阳能、电能以及热能对进一步提升NO_(3)RR性能的巨大潜力. 展开更多
关键词 铜光阴极 等离激元辅助电催化剂 光电效应 光热效应 硝酸根还原反应
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Recent progress in electrochemical synthesis of carbon-free hydrogen carrier ammonia and ammonia fuel cells:A review 被引量:1
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作者 Feng Du Wei Sun +1 位作者 Hui Luo Chang Ming Li 《Materials Reports(Energy)》 2022年第4期3-18,共16页
Ammonia(NH3)is a cornerstone widely used in the modern agriculture and industry,the annual global production gradually increases to almost 200 million tons.Nearly 80%of the produced NH3 is used in the fertilizer indus... Ammonia(NH3)is a cornerstone widely used in the modern agriculture and industry,the annual global production gradually increases to almost 200 million tons.Nearly 80%of the produced NH3 is used in the fertilizer industry and is essential for the development of global agriculture and consequently for maintaining population growth.Furthermore,NH3 can power hydrogen(H2)fueled devices,such as H2 fuel cells(FC),to use the interconversion between chemical energy and electric energy of nitrogen(N2)cycle,which can effectively alleviate the intermittent problems of renewable energy.However,the problems faced by NH3 in storage and release still restrict its development.Herein,this review introduces the latest research and development of electrochemical NH3 synthesis and direct NH3 FC,as well as outlines the technical challenges,possible improvement measures and development perspectives.N2 reduction reaction(NRR)and nitrate reduction reaction(NO3RR)are two potential approaches for electrochemical NH3 synthesis.However,the existing research foundation still faces challenges in achieving high selectivity and efficiency.Direct NH3 FC are easy to transport and are expected to be widely used in mobile energy consuming equipment,but also limited by the lack of highly active and stable NH3 oxidation electrocatalysts.The perspectives of ammonia fuel cells as an alternative green energy are discussed. 展开更多
关键词 Electrocatalysis Nitrogen reduction reaction(NRR) Nitrate reduction reaction(no3rr) Carbon-free hydrogen carrier Ammonia fuel cells
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