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Charge Redistribution Caused by S,P Synergistically Active Ru Endows an Ultrahigh Hydrogen Evolution Activity of S‐Doped RuP Embedded in N,P,S‐Doped Carbon
Advanced Science ( IF 14.3 ) Pub Date : 2020-07-20 , DOI: 10.1002/advs.202001526 Xiaoyu Liu 1 , Fan Liu 2 , Jiayuan Yu 2, 3 , Guowei Xiong 2 , Lili Zhao 2 , Yuanhua Sang 1 , Shouwei Zuo 4, 5 , Jing Zhang 4 , Hong Liu 1, 2 , Weijia Zhou 2
Advanced Science ( IF 14.3 ) Pub Date : 2020-07-20 , DOI: 10.1002/advs.202001526 Xiaoyu Liu 1 , Fan Liu 2 , Jiayuan Yu 2, 3 , Guowei Xiong 2 , Lili Zhao 2 , Yuanhua Sang 1 , Shouwei Zuo 4, 5 , Jing Zhang 4 , Hong Liu 1, 2 , Weijia Zhou 2
Affiliation
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Water splitting for production of hydrogen as a clean energy alternative to fossil fuel has received much attention, but it is still a tough challenge to synthesize electrocatalysts with controllable bonding and charge distribution. In this work, ultrafine S‐doped RuP nanoparticles homogeneously embedded in a N, P, and S‐codoped carbon sheet (S‐RuP@NPSC) is synthesized by pyrolysis of poly(cyclotriphosphazene‐co‐4,4′‐sulfonyldiphenol) (PZS) as the source of C/N/S/P. The bondings between Ru and N, P, S in PZS are regulated to synthesize RuS2 (800 °C) and S‐RuP (900 °C) by different calcination temperatures. The S‐RuP@NPSC with low Ru loading of 0.8 wt% with abundant active catalytic sites possesses high utilization of Ru, the mass catalytic activity is 22.88 times than 20 wt% Pt/C with the overpotential of 250 mV. Density functional theory calculation confirms that the surface Ru (−0.18 eV) and P (0.05 eV) are catalytic active sites for the hydrogen evolution reaction (HER), and the according charge redistribution of Ru is regulated by S and P with reverse electronegativity and electron–donor property to induce a synergistically enhanced reactivity toward the HER. This work provides a rational method to regulate the bonding and charge distribution of Ru‐based electrocatalysts by reacting macromolecules with multielement of C/N/S/P with Ru.
中文翻译：
S、P协同活性Ru引起的电荷重新分布赋予嵌入N、P、S掺杂碳中的S掺杂RuP超高的析氢活性
水分解制氢作为化石燃料的清洁能源替代品受到了广泛关注，但合成具有可控键合和电荷分布的电催化剂仍然是一个严峻的挑战。在这项工作中，通过聚（环三磷腈-co -4,4′-磺酰基联苯酚）的热解合成了均匀嵌入N、P和S共掺杂碳片中的超细S掺杂RuP纳米粒子（S-RuP@NPSC） （ PZS）作为C/N/S/P的来源。通过不同的煅烧温度调节PZS中Ru与N、P、S之间的键合，合成RuS 2 (800℃)和S-RuP(900℃)。Ru负载量为0.8 wt%的S-RuP@NPSC具有丰富的活性催化位点，Ru利用率高，质量催化活性是20 wt% Pt/C的22.88倍，过电位为250 mV。密度泛函理论计算证实，表面Ru（-0.18 eV）和P（0.05 eV）是析氢反应（HER）的催化活性位点，Ru相应的电荷重新分布受到具有反向电负性的S和P的调节，电子供体特性可诱导协同增强对 HER 的反应性。该工作提供了一种通过C/N/S/P多元素与Ru反应大分子来调节Ru基电催化剂的键合和电荷分布的合理方法。
更新日期：2020-09-10
中文翻译：
S、P协同活性Ru引起的电荷重新分布赋予嵌入N、P、S掺杂碳中的S掺杂RuP超高的析氢活性
水分解制氢作为化石燃料的清洁能源替代品受到了广泛关注，但合成具有可控键合和电荷分布的电催化剂仍然是一个严峻的挑战。在这项工作中，通过聚（环三磷腈-co -4,4′-磺酰基联苯酚）的热解合成了均匀嵌入N、P和S共掺杂碳片中的超细S掺杂RuP纳米粒子（S-RuP@NPSC） （ PZS）作为C/N/S/P的来源。通过不同的煅烧温度调节PZS中Ru与N、P、S之间的键合，合成RuS 2 (800℃)和S-RuP(900℃)。Ru负载量为0.8 wt%的S-RuP@NPSC具有丰富的活性催化位点，Ru利用率高，质量催化活性是20 wt% Pt/C的22.88倍，过电位为250 mV。密度泛函理论计算证实，表面Ru（-0.18 eV）和P（0.05 eV）是析氢反应（HER）的催化活性位点，Ru相应的电荷重新分布受到具有反向电负性的S和P的调节，电子供体特性可诱导协同增强对 HER 的反应性。该工作提供了一种通过C/N/S/P多元素与Ru反应大分子来调节Ru基电催化剂的键合和电荷分布的合理方法。
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