ORR催化剂Ni_m@Pt_1Au_(n-m-1)(n=19,38,55,79;m=1,6,13,19)的密度泛函研究（英文）

燃料电池的阴极反应的反应动力学速率非常慢,限制了燃料电池技术的发展。因此,寻找低成本、高活性的氧还原催化剂具有重要的意义。多元金属核壳团簇表现出优良的氧还原活性。在本文中,以原子个数为19、38、55和79的八面体团簇作催化剂模型,采用密度泛函理论(GGA-PBE-PAW)方法,研究了一系列不同尺寸核壳Ni_m@M_(n-m)(n=19, 38, 55, 79;m=1, 6,13, 19; M=Pt, Pd, Cu, Au, Ag)团簇催化剂的活性规律。优化*O、*OH和*OOH吸附中间体结构,计算了吸附自由能和反应吉布斯自由能,以超电势为催化活性的描述符,研究了单原子Pt嵌入Ni_m@Au_(n-m)团簇的活性规律。结果表明,Ni_6@Pt_1Au_(31)具有最好的ORR活性,并且Ni_1@Pt_1Au_(17)、Ni_6@Pt_1Au_(31)、Ni_(13)@Pt_1Au_(41)、Ni_(19)@Pt_1Au_5表现出比Pt_(38)团簇以及Pt(111)表面更高的催化活性。Bader电荷和态密度分析表面,核壳之间的电荷转移以及单原子Pt嵌入Ni_m@Au_(n-m)表面,改变了吸附位的电子性质,降低了*OH的吸附强度,提高了ORR活性。单原子Pt嵌入Ni_m@Au_(n-m)表面可能是一种合适的多元金属核壳ORR催化剂设计策略。     

碱土金属Ben (n=1~3)对B12团簇结构的调控研究

基于第一性原理, 系统地研究了Be_n (n=1~3)对B₁₂团簇结构的调控. 结果表明: 团簇BeB₁₂全局极小结构为C_s对称性准平面结构, 而Be₂B₁₂和Be₃B₁₂最稳定的结构均为笼状结构, 对称性分别为C_s和C_2v. 随着Be_n (n=1~3)原子数的增加, 团簇B₁₂由准平面结构过渡到笼状结构, 且Be倾向内嵌在B₁₂笼状结构表面的B₇或B₈单元环中, 通过离子和共价作用形成稳定Be&B₇和Be&B₈单元, 从而稳定笼状结构. 自然键轨道(NBO)分析表明, 团簇C_s BeB₁₂, C_s Be₂B₁₂, C_2v Be₃B₁₂内部存在电子转移情况, Be原子2s轨道上失去电子, Be—B键主要以离子作用为主, 同时也存在共价作用. 成键分析显示C_s Be₂B₁₂和C_2v Be₃B₁₂的π键遵循球状芳香性2(n+1)² (n=1)电子计数规则, 表明该团簇具有球状芳香性. 预测了三个结构的红外和拉曼光谱, 为以后的合成实验和数据表征提供了理论基础.     

核-壳结构多酸/磁性铈铁纳米复合氧化物@SiO2吸附-氧化脱硫性能

水热法合成了铈铁纳米复合氧化物,采用化学沉积法在其表面包裹SiO₂制备核-壳结构磁性材料,以其为载体负载H₂O₂结合Keggin结构磷钼酸(HPMo)制备了HPMo-H₂O₂/CeFe_xO_y@SiO₂吸附-氧化脱硫催化剂。 采用扫描电子显微镜(SEM)、透射电子显微镜(TEM)、傅里叶红外光谱(FT-IR)、X射线粉末衍射(XRD)、氮气吸附脱附(BET)、³¹P魔角核磁共振(MAS-NMR)和X射线光电子能谱(XPS)等对催化剂的结构进行表征。 结果表明,SiO₂将CeFe_xO_y包裹形成核-壳结构纳米复合材料,以其为载体负载HPMo-H₂O₂后Keggin型多酸的骨架结构保持,并产生少量过氧化磷钼酸盐活性物种。 不同催化剂对有机硫化物二苯并噻吩(DBT)的吸附脱硫和氧化脱硫性能,均呈现出HPMo-H₂O₂/CeFe_xO_y@SiO₂＞CeFe_xO_y@SiO₂＞CeFe_xO_y的活性顺序,多酸的引入大大提升了其对大分子有机硫化物的吸附和氧化脱除性能,催化氧化脱硫活性的提高源于多酸分子“假液相”反应过程的结果。 在反应温度60 ℃,反应3 h,m(油)∶m(催化剂)=35∶1,n(O)∶n(S)=10∶1的条件下,对DBT氧化脱除率达到99.4%。 制备的磁性核-壳结构氧化脱硫剂有理想的氧化脱除DBT的循环使用性能,并且可通过外加磁场进行简单分离,是一类制备方法简单、催化活性高且稳定性好的绿色环保型催化剂。     

Keggin型多酸负载的单原子催化剂(M1/POM,M = Ni,Pd, Pt,Cu, Ag,Au, POM = [PW12O40]3-)活化氮气分子的密度泛函理论计算研究

采用量子化学密度泛函理论(DFT)结合自然键轨道(NBO)分析的方法对一系列以多酸为载体的单原子催化剂(SACs)(M₁/POM (M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-)的分子几何、电子结构及红外光谱进行计算。结果表明,Pt₁/POM对N₂分子具有潜在的活化能力,Pt₁/POM与N₂相互作用主要来自于由金属Pt的d_xz和d_yz轨道与N₂的π^*反键轨道重叠,金属Pt的d_xz、d_yz轨道上的电子填充到了氮气的π^*反键轨道上弱化了N≡N成键,导致了N≡N之间的键长增大,有效的活化了氮气分子。对它们红外光谱的分析表明,Keggin型多酸负载金属后W―O_c―W振动吸收峰发生劈裂,产生了五个典型的红外特征吸收峰。     

中性团簇(CeO2)m(m=1~3)活化甲烷C—H的密度泛函理论计算

采用密度泛函理论(DFT)计算了CH₄在电中性(CeO₂)_m(m=1~3)团簇上的活化情况, 并对其机理进行了探讨. 计算结果表明, 甲烷C—H键在团簇上的活化为亲核加成模式, 电子由团簇流向甲烷C—H反键轨道, 使甲烷C—H键削弱而得以活化, 反应的过渡态为四中心结构. 团簇的桥氧位活化甲烷C—H键的活性大于端氧位, 而三重桥氧位的活性高于二重桥氧位. 团簇中作用位点Ce和O原子的电荷布居与其活化甲烷C—H的能力密切相关. 溶剂的存在不仅降低了甲烷C—H活化自由能垒, 而且使与甲烷作用的团簇各位点的活性差异缩小.     

Keggin型杂多酸铯盐催化苯羟基化反应

采用室温固相法制备了具有Keggin结构的杂多酸铯盐催化剂(Cs_xH_3+n-xPMo_12-nV_nO₄₀, n＝0, 1, 2, x＝0.5～3.0). 红外、X射线粉末衍射及循环伏安技术研究显示, 钒取代钼原子可提高催化剂的氧化还原性, 铯取代数的增加可提高催化剂的疏水性但降低氧化还原性. 在H₂O₂为氧化剂的苯羟基化反应中, 随着铯取代数目的增加, 催化剂的溶脱情况得到明显改善. 在氧化还原性和疏水性协同作用下, Cs₂H₃PMo₁₀V₂O₄₀在Cs_xH_3+n-xPMo_12-nV_nO₄₀系列催化剂中显示出相对最佳的苯羟基化催化活性(苯酚收率19.2%)和重复使用性能.     

Cu掺杂对Pt/Ba/CuxMg1-xAl2O4催化剂高温稀燃NOx消除性能的影响

制备了一系列不同Cu掺杂量的Pt/Ba/Cu_xMg_1-xAl₂O₄(x=0, 0.1, 0.3)催化剂, 将其应用于高温NO_x储存还原(NSR)反应, 并探究了Cu掺杂量对催化剂NO_x消除性能的影响. 结果表明, 储存组分BaCO₃在NSR过程中存在再分散现象. 高温时催化剂的NO_x消除性能取决于其NO_x储存量, 而不是NO氧化和NO_x还原性能. 高温时催化剂的NO_x储存量与其上硝酸盐的热稳定性密切相关, Pt/Ba/MgAl₂O₄上NO_x主要以离子态硝酸盐形式存在, 而掺杂Cu后催化剂上的NO_x又增加了单齿硝酸盐的存在形式, 单齿硝酸盐具有更高的热稳定性, 因此掺Cu催化剂具有更大的NO_x储存量. 在450~500 ℃范围内, Cu的掺杂显著提高了Pt/Ba/MgAl₂O₄的NO_x消除性能; Pt/Ba/Cu_0.1Mg_0.9Al₂O₄催化剂的性能最佳, 450 ℃时的NO_x消除效率高达90%.     

纳米尺寸氧化钇团簇阴离子与正丁烷反应的研究

在单一原子量分辨水平上研究纳米尺寸过渡金属氧化物团簇(M_xO_y^q)与小分子的反应不仅能够获得氧化物纳米颗粒的反应性随原子组成和尺寸连续变化的演变规律, 而且对认识其结构特征以及表面活性氧物种(如O^-•自由基)的产生机制等具有重要意义. 本工作分别采用耦合快速流动反应管和耦合四极质量过滤器-线形离子阱的两套反射式飞行时间质谱研究了不同“氧缺陷指数”(Δ)的氧化钇团簇Y_xO_y^- (x≤50,y≤76; Δ≡2y–1–3x, Δ=0~5)和掺杂氟(F)原子团簇Y _xO_yF^- [x≤49,y≤74; Δ≡(2y+1)–1–3x, Δ=1]与 n-C₄H₁₀分子的反应. 实验观测到Δ=1系列团簇(Y₂O₃)_NO^- (N=1~25)、(Y₂O₃)_NYO₂F^- (N=1~24)及Δ=4系列团簇(Y₂O₃)_NYO₄^- (N=1, 3~24)具有氢抽取反应活性, N≥2时其它Δ系列团簇(Δ=0, 2, 3, 5)在相同实验条件下没有表现出明显的反应性. 密度泛函理论研究Δ=1或4系列小尺寸团簇(Y₂O₃)_NY_xO_yF_0,1^- (N≤4;x=0, 1)的结构揭示O^-•自由基是氢抽取反应的活性位点, 结合实验可推测Δ=1或4系列纳米尺寸团簇(Y₂O₃)_NY_xO_yF_0,1^- (x=0, 1)结构中也含有O^-•自由基. 这些结果表明Δ=0系列惰性纳米尺寸团簇(Y₂O₃)_NYO₂^-可以通过吸附一个O₂分子发生电子转移生成O^-•自由基(O^2-+O₂→O^-•+O₂^-•), 也可以通过掺入F原子的方式生成O^-•自由基(O^2-+F^•→O^-•+F^-).     

高指数晶面和梯度组成的PtCu3@Pt3Cu@Pt纳米枝晶氧还原电催化剂性能

燃料电池作为一种清洁、高效的能量转换装置,其大规模应用受到阴极氧还原反应(ORR)动力学缓慢以及铂资源稀缺和价格高昂等的极大制约.尽管研究人员在过去几十年中付出了巨大努力,但研制高效、耐用的低Pt合金催化剂仍亟待突破.近年的研究表明,Pt的一些高指数晶面能够表现出比Pt(111)晶面更高的ORR活性,尤其是Pt(332),Pt(331)和Pt(554)等.同时,合金化能够通过电子与几何效应减弱含氧物种在Pt表面的吸附能,提升Pt合金催化剂的ORR活性.因此,高指数晶面和合金化的结合将是设计开发高性能电催化剂的有效手段.本文提出一种气氛调控的液相合成方法,通过在油胺中加热还原Pt化合物和Cu化合物,不添加其它保护剂,仅通过反应气氛的调控,成功制备了不同形貌的Pt-Cu合金纳米结构(纳米多脚、纳米凹立方体、纳米枝晶).通过反应前期引入氧化性气氛随后切换为惰性气氛的调控策略,合成具有高指数晶面的具有纳米枝晶结构的PtCu3合金;进一步对其进行电化学去合金化形成富Pt壳层,既保持其纳米枝晶形貌和高指数晶面,又形成具有梯度组成的PtCu₃@Pt₃Cu@Pt纳米枝晶.相比而言,全程惰性气氛下生长得到纳米多脚结构,全程氧化性气氛下生长则得到纳米凹立方体.电化学测试结果表明,在0.1 M HClO4电解液中,PtCu₃@Pt₃Cu@Pt纳米枝晶展现出较高的ORR活性,在0.9 V(vs.RHE)处的Pt质量活性和面积活性高达1.55 A mgPt^-1和2.4 mA cmPt^-2,分别为商业Pt/C催化剂的14倍和24倍;此外,PtCu₃@Pt₃Cu@Pt纳米枝晶具有良好的电化学稳定性能,经0.7~1.1 V(vs.RHE)电势范围内循环5000圈,其催化活性保持稳定.DFT计算表明,Cu合金效应和高指数晶面结构共同增强了Pt的ORR活性,其中PtCu₃@Pt₃Cu@Pt纳米枝晶高指数晶面台阶位点的氧结合能接近最优值,从而表现出火山顶点附近的ORR活性.     

Rh@Pt内凹立方体核壳催化剂的制备及其乙醇电氧化性能

贵金属Rh基催化剂可有效催化乙醇中C―C键断裂,有利于实现乙醇完全电氧化,但Rh催化剂对乙醇电氧化的催化活性较低。本文通过种子介导生长法制备了具有内凹立方体形貌的Rh@Pt/C核壳催化剂,考察了不同Pt壳层厚度的Rh@Pt/C核壳催化剂在碱性介质中对乙醇电氧化反应(EOR)的催化性能。其中Rh@Pt_0.25/C核壳催化剂对EOR的质量归一化电流最高为520 mA/mg,此时面积归一化电流也最高,为0.16 mA/cm²。研究表明,Rh@Pt/C核壳催化剂中Rh和Pt之间的表面应变效应和电子配体效应取决于Rh表面Pt壳层的厚度,Pt壳层厚度的改变,可调控催化剂中Rh和Pt的协同作用,从而减弱毒性中间体对催化剂表面的吸附,优化催化剂对EOR的性能。总体上,Rh表面Pt壳层为3层的Rh@Pt_0.25/C核壳催化剂表现出最优的EOR活性和稳定性,此时催化剂也兼具了较优的抗毒化能力。     

高活性和高稳定性的核壳结构PtPx@Pt/C催化氧还原

在质子交换膜燃料电池中,金属铂是最高效的阴极氧还原催化剂之一,但是铂昂贵的价格严重阻碍了其在燃料电池领域中的大规模商业化应用.通过铂与3d过渡金属(Fe、Co和Ni)合金化可以有效提高催化剂的氧还原活性,然而在实际的高腐蚀性、高电压和高温的燃料电池运行环境中,铂合金纳米粒子易发生溶解、迁移和团聚,从而导致催化剂耐久性差.同时过渡金属离子的溶出会影响质子交换膜的质子传导,并且一些过渡金属离子会催化芬顿反应,产生高腐蚀性?OH自由基,加快Nafion和催化剂的劣化.与过渡金属掺杂相比,非金属掺杂具有明显优势:一方面,非金属溶出产生的阴离子不会取代Nafion中的质子,也不会催化芬顿反应;另一方面,与3d过渡金属相比,非金属具有更高的电负性,其掺杂很容易调节Pt的电子结构.因此,本文通过非金属磷掺杂合成具有优异稳定性的核壳结构PtPx@Pt/C氧还原催化剂.通过热处理磷化商业碳载铂形成磷化铂(PtP2),经由酸洗处理产生富铂壳层,即PtPx@Pt/C.X射线粉末多晶衍射结果证明了PtP2相的存在,并且进一步通过电子能量损失谱对纳米粒子进行微区面扫描分析以及X射线光电子能谱分析证实了富铂壳层的存在,壳层厚度约1 nm.得益于核壳结构及磷掺杂引起的电子结构效应,PtP1.4@Pt/C催化剂在0.90 V(RHE)时的面积活性(0.62 mA cm–2)与质量活性(0.31 mAμgPt–1)分别是商业Pt/C的2.8倍和2.1倍.更重要的是,在加速耐久性测试中,PtP1.4@Pt/C催化剂在30000圈电位循环后质量活性仅衰减6％,在90000圈电位循环后仅衰减25％;而商业Pt/C催化剂在30000圈电位循环后就衰减46％.PtP1.4@Pt/C催化剂高活性与高稳定性主要归功于核壳结构、磷掺杂引起的电子结构效应以及磷掺杂增加了碳载体对催化剂粒子的锚定作用进而阻止了其迁移团聚.综上所述,本文为设计同时具有优异活性与稳定性非金属掺杂Pt基氧还原催化剂提供新的思路.     

Highly active Pt@Au nanoparticles encapsulated in perfluorosulfonic acid for the reduction of oxygen

The Pt@Au catalysts demonstrate remarkably high oxygen reduction reaction (ORR) activity compared with Pt/C catalysts. The ORR of Pt(2)@Au(1)/C and Pt(1)@Au(2)/C is 9.5 and 6.6 times that of Pt/C, respectively. This improvement is attributed to the electronic structure effect of the Au core on the Pt shell and introduction of PFSA.     

Icosahedral platinum alloy nanocrystals with enhanced electrocatalytic activities

This communication describes the synthesis of Pt-M (M = Au, Ni, Pd) icosahedral nanocrystals based on the gas reducing agent in liquid solution method. Both CO gas and organic surface capping agents play critical roles in stabilizing the icosahedral shape with {111} surfaces. Among the Pt-M alloy icosahedral nanocrystals generated, Pt(3)Ni had an impressive ORR specific activity of 1.83 mA/cm(2)(Pt) and 0.62 A/mg(Pt). Our results further show that the area-specific activity of icosahedral Pt(3)Ni catalysts was about 50% higher than that of the octahedral Pt(3)Ni catalysts (1.26 mA/cm(2)(Pt)), even though both shapes are bound by {111} facets. Density functional theory calculations and molecular dynamics simulations indicate that this improvement may arise from strain-induced electronic effects.     

Single‐Atom Iron Catalysts on Overhang‐Eave Carbon Cages for High‐Performance Oxygen Reduction Reaction

Single‐atom catalysts have drawn great attention, especially in electrocatalysis. However, most of previous works focus on the enhanced catalytic properties via improving metal loading. Engineering morphologies of catalysts to facilitate mass transport through catalyst layers, thus increasing the utilization of each active site, is regarded as an appealing way for enhanced performance. Herein, we design an overhang‐eave structure decorated with isolated single‐atom iron sites via a silica‐mediated MOF‐templated approach for oxygen reduction reaction (ORR) catalysis. This catalyst demonstrates superior ORR performance in both alkaline and acidic electrolytes, comparable to the state‐of‐the‐art Pt/C catalyst and superior to most precious‐metal‐free catalysts reported to date. This activity originates from its edge‐rich structure, having more three‐phase boundaries with enhanced mass transport of reactants to accessible single‐atom iron sites (increasing the utilization of active sites), which verifies the practicability of such a synthetic approach.     

钴原子团簇用于高效氧还原反应

探索非贵金属材料作为高效氧还原反应催化剂是迫切需要的，但具有一定的挑战性。本文采用等离子体轰击和酸洗相结合的策略合成了Co原子团簇修饰的多孔碳载体催化剂(Co_AC/NC)。通过多种表征手段证实了的原子团簇特征。所得到的Co_AC/NC催化剂在三电极体系和锌-空电池方面都表现出优异的氧还原反应活性。该催化剂的氧还原反应半波电位为0.887 V，显著优于商业Pt/C催化剂，且表现出优异的稳定性。此外，该催化剂组装的锌-空电池的峰值功率密度为181.5 mW∙cm⁻²，同样远高于Pt/C催化剂。这项工作不仅合成了一种高效的氧还原反应催化剂，而且为原子团簇催化剂的理性设计和实际应用提供了新的见解。     

Recent advances in carbon-based electrocatalysts for oxygen reduction reaction

Fuel cells are one of the most promising clean energy devices to substitute for fossil fuel in the future to alleviate energy crisis and environmental pollution.As the key reaction on the cathode in the fuel cells,oxygen reduction reaction(ORR)still requires efficient noble metal catalysts such as the comme rcial Pt/C to boost the reaction for its sluggish kinetics.Therefore,it is critical to design earth-abundant carbonbased catalysts with high efficiency and long-term stability to replace the noble metal-based catalysts.This review focuses on the recent progress about carbon-based ORR catalysts including non-metal doped carbon materials,transition metal-nitrogen-carbon species,transition metal carbides/carbon,single atom catalysts,and other carbon hybrids.And we further infer that the excellent ORR performances can be achieved by the balance of geometric and electronic structures of catalysts such as conductivity,surface area,hierarchical porous structure,defect and doping effect.Additionally,the perspective development trend is also proposed to guide the rational designation of carbon-based catalysts for ORR and even extend to other energy storage and conversion fields in the future.     

Geometric, electronic, and bonding properties of AuNM (N = 1-7, M = Ni, Pd, Pt) clusters

Employing first-principles methods, based on density functional theory, we report the ground state geometric and electronic structures of gold clusters doped with platinum group atoms, Au(N)M (N = 1-7, M = Ni, Pd, Pt). The stability and electronic properties of Ni-doped gold clusters are similar to that of pure gold clusters with an enhancement of bond strength. Due to the strong d-d or s-d interplay between impurities and gold atoms originating in the relativistic effects and unique properties of dopant delocalized s-electrons in Pd- and Pt-doped gold clusters, the dopant atoms markedly change the geometric and electronic properties of gold clusters, and stronger bond energies are found in Pt-doped clusters. The Mulliken populations analysis of impurities and detailed decompositions of bond energies as well as a variety of density of states of the most stable dopant gold clusters are given to understand the different effects of individual dopant atom on bonding and electronic properties of dopant gold clusters. From the electronic properties of dopant gold clusters, the different chemical reactivity toward O(2), CO, or NO molecule is predicted in transition metal-doped gold clusters compared to pure gold clusters.     

Epoxy-rich Fe Single Atom Sites Boost Oxygen Reduction Electrocatalysis

Electrocatalysts for highly efficient oxygen reduction reaction (ORR) are crucial for energy conversion and storage devices. Single-atom catalysts with maximized metal utilization and altered electronic structure are the most promising alternatives to replace current benchmark precious metals. However, the atomic level understanding of the functional role for each species at the anchoring sites is still unclear and poorly elucidated. Herein, we report Fe single atom catalysts with the sulfur and oxygen functional groups near the atomically dispersed metal centers (Fe1/NSOC) for highly efficient ORR. The Fe1/NSOC delivers a half-wave potential of 0.92 V vs. RHE, which is much better than those of commercial Pt/C (0.88 V), Fe single atoms on N-doped carbon (Fe1/NC, 0.89 V) and most reported nonprecious metal catalysts. The spectroscopic measurements reveal that the presence of sulfur group induces the formation of epoxy groups near the FeN4S2 centers, which not only modulate the electronic structure of Fe single atoms but also participate the catalytic process to improve the kinetics. The density functional theory calculations demonstrate the existence of sulfur and epoxy group engineer the charges of Fe reactive center and facilitate the reductive release of OH* (rate-limiting step), thus boosting the overall oxygen reduction efficiency.     

表面修饰型铂基氧还原电催化剂研究进展

氧气还原反应是燃料电池中的重要电极反应,但其动力学过程非常迟缓,需高度依赖资源稀缺、价格高昂的贵金属Pt。加之Pt基催化剂还面临着实际工况下耐久性不足的问题,这些都严重阻碍了燃料电池的产业化进程。对Pt基纳米催化剂进行表面功能化修饰可有效优化和提升其氧还原活性和稳定性。本文综述了最近几年表面修饰型Pt基氧还原催化剂的最新研究,着重探讨了表面修饰物的选择、表面修饰的手段和策略以及表面修饰前后对催化剂氧还原性能的影响,并指出该类型催化剂未来发展方向。     

Designing high performance Pt monolayer core–shell electrocatalysts for fuel cells

In proton exchange membrane fuel cells, platinum (Pt) has been the dominant choice for both the cathode and the anode catalysts. The high Pt content and high associated costs particularly at the cathode, and sluggish oxygen reduction reaction (ORR) kinetics and poor stability, remain a challenge. Pt monolayer (ML) catalysts offer a distinctively reduced Pt content while providing considerable possibilities for enhancing their catalytic activity and stability for the ORR. In this opinion, we first review the achievement in active and stable Pt ML on palladium (Pd) nanoparticle catalysts for the ORR. We then describe the mechanisms that rationalize their high activity and durability. Recently, we developed several novel nanostructured cores to further improve the ORR activity and stability by optimizing their surface orientation, composition, and morphology. The results from the Pt ML catalysts significantly impact the research of electrocatalysis and fuel-cell technology, as they demonstrate an exceptionally effective way of design and syntheses of catalysts.