MoP-NC纳米球负载Pt纳米粒子用于高效甲醇电解.pdf
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1、物 理 化 学 学 报 Acta Phys.-Chim.Sin.2023,39(9),2301005(1 of 10)Received:January 3,2023;Revised:February 7,2023;Accepted:February 8,2023;Published online:February 24,2023.*Corresponding author.Email:;Tel.:+86-17306299692.The project was supported by the National Natural Science Foundation of China(219721
2、24,22102105,22272148).国家自然科学基金(21972124,22102105,22272148)资助项目 Editorial office of Acta Physico-Chimica Sinica Article doi:10.3866/PKU.WHXB202301005 MoP-NC Nanosphere Supported Pt Nanoparticles for Efficient Methanol Electrolysis Meng Li 1,Fulin Yang 1,Jinfa Chang 2,Alex Schechter 3,Ligang Feng 1,*1
3、 School of Chemistry and Chemical Engineering,Yangzhou University,Yangzhou 225002,Jiangsu Province,China.2 NanoScience Technology Center,University of Central Florida,Orlando,FL 32826,USA.3 Department of Chemical Sciences,Ariel University,Ariel 40700,Israel.Abstract:Hydrogen energy is a potential en
4、ergy storage carrier due to its advantages of cleanliness,high efficiency and renewability.Electrocatalytic water splitting is an ideal method to generate hydrogen,and the slow kinetics of water oxidation,namely,oxygen evolution reaction(OER),greatly restricts its practical application.To reduce the
5、 energy consumption required for OER,methanol oxidation reaction(MOR)with a much lower theoretical potential is very promising to replace OER to assist hydrogen generation.The theoretical potential of MOR is only 0.016 V vs.SHE(standard hydrogen electrode),which is much lower than that of OER(1.23 V
6、),and the energy-saving can be about 60%compared to that of traditional water electrolysis.Therefore,using MOR instead of OER to realize methanol electrolysis for hydrogen production is an effective way to reduce energy consumption.An efficient bifunctional catalyst is very important for green hydro
7、gen generation from overall methanol electrolysis.Currently,Pt-based materials are still the best catalyst for hydrogen evolution reaction(HER)and MOR,while they are more challenging in the MOR as they are prone to intermediates poisoning during the catalytic reactions.The introduction of transition
8、 metal-based promoters such as phosphides is an effective strategy to promote the catalytic ability for methanol oxidation.Herein,ultrafine Pt nanoparticles with an average particle size of 2.53 nm evenly grown on MoP-NC nanosphere(Pt/MoP-NC)were demonstrated as an efficient electrocatalyst for meth
9、anol electrolysis towards hydrogen generation.The introduction of MoP-NC nanospheres support not only restricts the aggregation of Pt,but also improves the catalytic performance and anti-poisoning ability.Specifically,Pt/MoP-NC catalyst exhibited high methanol oxidation performance with a peak curre
10、nt density of 90.7 mAcm2,which was 3.2 times higher than that of commercial Pt/C catalysts,and good hydrogen evolution reaction performance with a low overpotential of 30 mV to offer 10 mAcm2 in an acid medium,which was comparable to commercial Pt/C.The assembled Pt/MoP-NC|Pt/MoP-NC electrolyzer sho
11、wed a cell voltage of 0.67 V at 10 mAcm2,ca.1.02 V less than that of the overall water splitting system(1.69 V).The high catalytic ability of Pt/MoP-NC originated from the electronic effect between noble metal active center Pt and the adjacent MoP-NC support with a unique layered porous spherical st
12、ructure.The partial electron transfer from MoP to Pt can lower the d-energy band center of Pt,which weakened the binding energy between Pt and adsorbed toxic intermediates.In addition,the oxophilic MoP-NC nanospheres can activate water to provide more hydroxyl species and facilitate the oxidative re
13、moval of CO intermediates adsorbed on the Pt active sites.The current work might inspire the design and preparation of novel catalyst platforms for methanol electrolysis in hydrogen generation.Key Words:Electronic effect;Methanol electrolysis;Transition metal phosphides;Platinum-based catalyst;Bifun
14、ctional catalyst 物理化学学报 Acta Phys.-Chim.Sin.2023,39(9),2301005(2 of 10)MoP-NC 纳米球负载纳米球负载 Pt 纳米粒子用于高效甲醇电解纳米粒子用于高效甲醇电解 李萌1,杨甫林1,常进法2,Alex Schechter 3,冯立纲1,*1扬州大学化学化工学院,江苏 扬州 225002 2 NanoScience Technology Center,University of Central Florida,Orlando,FL 32826,USA.3 Department of Chemical Sciences,Arie
15、l University,Ariel 40700,Israel.摘要:摘要:实现绿色甲醇电解制氢需要高效的双功能催化剂。本文采用热处理结合乙二醇还原法成功制备了MoP-NC纳米球负载的超细Pt纳米粒子(平均粒径为2.53 nm)复合催化剂(Pt/MoP-NC)用于高效甲醇电解制氢。MoP-NC纳米球不仅能提高Pt纳米粒子的分散性并且增强Pt的抗中毒能力。电化学测试表明Pt/MoP-NC催化剂在酸性甲醇氧化反应(MOR)和析氢反应(HER)中具有较高的催化性能;其中,MOR的正向扫描峰值电流密度为90.7 mAcm2,是商业Pt/C催化剂的3.2倍,在10 mAcm2的电流密度下,HER的过电位
16、低至30 mV,与商业Pt/C接近。由Pt/MoP-NC|Pt/MoP-NC组装的两电极电解槽驱动10 mAcm2的电流密度仅需要0.67 V的电压,比相同条件下电解水的电压低1.02 V,大大降低了能量输入。Pt/MoP-NC的高催化性能主要来源于Pt活性中心与相邻层状多孔球形结构的MoP-NC载体之间电子效应及配体效应引起的抗一氧化碳中毒能力的提升和含氧物种的容易生成。关键词:关键词:电子效应;甲醇电解;过渡金属磷化物;铂基催化剂;双功能催化剂 中图分类号:中图分类号:O646 1 Introduction The energy crisis induced by a large amou
17、nt of fossil fuel consumption has accelerated the development of sustainable and environment-friendly energy sources such as solar,and wind energy 14.While the intermittence of these energies cannot meet the practical application,and thus,they should be transferred to proper energy for storage 5,6.H
18、ydrogen as a recyclable and clean energy is considered the best form,which can be produced by these sustainable energies via the water splitting technique.Therefore,electrochemical water splitting for hydrogen production has received much attention 7,8.The thermodynamic potential for water splitting
19、 is 1.23 V under standard conditions,and much higher energy input is required due to the high overpotentials generated during the electrocatalysis,especially for the complicated and sluggish anode oxygen evolution reaction(OER)9,10.To reduce the overpotential and make the whole reaction more energy
20、efficient,an effective approach was proposed to replace the OER with an alternative reaction that can happen at low potentials 11,12.Among the possible reactions 1315,methanol oxidation,which has a thermodynamic potential of 0.016 V,has been demonstrated very promising to replace OER;and the corresp
21、onding methanol electrolysis would be more competitive for hydrogen generation,as claimed that the energy-saving can be about 60%compared to that of traditional water electrolysis 16,17.To realize efficient methanol electrolysis,high-performing catalysts are required to catalyze the methanol oxidati
22、on reaction(MOR)and hydrogen evolution reaction(HER)for methanol electrolysis 18.The Pt-based materials are still the best catalyst for these reactions 19,while it is more challenging in the MOR as they are vulnerable to intermediates poisoning during the catalytic reactions 2022.So,attention should
23、 be directed to the anode catalyst study;currently,it is an effective strategy to promote methanol oxidation of Pt by introducing transition metal-based promoters such as oxides and phosphides 22,23.For example,Pt/C/TiO2 catalyst showed good catalytic activity for MOR due to strong metal-support int
24、eractions between Pt nanoparticles and TiO2 nanotubes 24;in addition,TiO2 nanotubes could activate water to provide adsorbed OH intermediates(OHads)species in assisting the poisoning adsorbed CO intermediates(COads)removal on Pt sites via a bi-functional catalytic mechanism.The better CO tolerance o
25、f the Pt/FeP nanosheet hybrid was also attributed to the cooperative effect from the down-shifted d-band center of Pt induced by the special activity of Fe+and P 25.Molybdenum phosphide(MoP)has received special attention for water adsorption and dissociation due to the different electronegativities
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