摘要：Electrocatalytic nitrate reduction reaction is considered as a promising and sustainable method for ammonia ***,the selectivity and yield rate of ammonia are limited by the competitive hydrogen evolution reaction and the complex eight-electron transfer ***,we developed a(FeCoNiCu)Ox/CeO_(2)polymetallic oxide electrocatalyst for effective nitrate reduction to *** synergistic effects among the multiple elements in the electrocatalyst were clearly elucidated by comprehensive ***,Cu acted as the active site for reducing nitrate to nitrite,and Co facilitated the subsequent reduction of nitrite to ammonia,while Fe and Ni promoted water dissociation to provide ***,the incorporation of CeO_(2)increased the active surface area of(FeCoNiCu)Ox,resulting in an improved ammonia yield rate to meet industrial ***,the(FeCoNiCu)Ox/CeO_(2)electrocatalyst achieved an ammonia current density of 382 mA cm^(-2)and a high ammonia yield rate of 30.3 mg h^(-1)cm^(-2)with a long-term *** work offers valuable insights for the future design of highly efficient multi-element electrocatalysts.

摘要：The design and synthesis of high‐performance and low‐cost electrocatalysts for the hydrogen evolution reaction(HER),a key half‐reaction in water electrolysis,are *** to their modest hydrogen adsorption energy,ruthenium(Ru)‐based nanomaterials are considered outstanding candidates to replace the expensive platinum(Pt)‐based HER *** this study,we developed an adsorption‐pyrolysis method to construct nitrogen(N)‐doped graphene aerogel(N‐GA)‐supported ultrafine Ru nanocrystal(Ru‐NC)nanocomposites(Ru‐NCs/N‐GA).The particle size of the Ru‐NCs and the conductivity of the N‐GA substrate can be controlled by varying the pyrolysis *** experiments reveal revealed that 10 wt%Ru‐NCs/N‐GA nanocomposites require overpotentials of only 52 and 36 mV to achieve a current density of 10 mA cm^(−2) in 1 mol/L HClO4 and 1 mol/L KOH electrolytes for HER,respectively,which is comparable to 20 wt%Pt/C *** from the ultrafine size and uniform dispersion of the Ru‐NCs,the synergy between Ru and the highly conductive substrate,and the anchoring effect of the N atom,the Ru‐NCs/N‐GA nanocomposites exhibit excellent activity and durability in the pH‐universal HER,thereby opening a new avenue for the production of commercial HER electrocatalysts.

摘要：Rational composition design of trimetallic phosphide catalysts is of significant importance for enhanced surface reaction and efficient catalytic ***,hierarchical Co_(x)Ni_(y)Fe_(z)P with precise control of stoichiometric metallic elements(x:y:z=(1-10):(1-10):1)has been synthesized,and Co_(1.3)Ni_(0.5)Fe_(0.2)P,as the most optimal composition,exhibits remarkable catalytic activity(η=320 mV at 10 mA cm^(−2))and long-term stability(ignorable decrease after 10 h continuous test at the current density of 10 mA cm^(−2))toward oxygen evolution reaction(OER).It is found that the surface P in Co_(1.3)Ni_(0.5)Fe_(0.2)P was replaced by O under the OER *** density function theory calculations before and after long-term stability tests suggest the clear increasing of the density of states near the Fermi level of Co_(1.3)Ni_(0.5)Fe_(0.2)P/Co_(1.3)Ni_(0.5)Fe_(0.2)O,which could enhance the OH−adsorption of our electrocatalysts and the corresponding OER performance.

摘要：将甲烷直接转化为燃料和高附加值化学品引起了越来越多的研究兴趣,然而由于甲烷的化学惰性,实现这一过程仍然是一个巨大的挑战.本文设计了12种单原子合金催化剂(SAAs)应用于甲烷的活化,利用密度泛函理论(DFT)计算和微观动力学模拟筛选出对甲烷C–H键解离具有优异催化活性的单原子合金,并在此基础上进一步研究了甲烷选择性氧化制甲醇的机理.计算结果表明,惰性金属Ag、Au和Cu基底中掺杂Ir单原子具有更高的甲烷解离活性,这主要源于甲烷C–H键与Ir原子投影d轨道之间的相互作用.在引入分子氧之后,我们提出了甲烷选择性氧化制甲醇的三种反应机理.通过DFT计算确定了3条途径的完整反应网络,同时微观动力学模拟揭示了实际反应条件下每种SAA表面上反应物种覆盖度的变化.表面覆盖度分析表明,在所有的温度范围内,Ir1/Ag表面都有利于氧化反应,而Ir1/Au和Ir1/Cu只在有限的温度区间内有利于该氧化过程,表明Ir1/Ag单原子合金是甲烷选择性氧化制甲醇反应中非常有效的单原子合金催化剂.

摘要：Developing efficient platinum(Pt)-based electrocatalysts is enormously significant for fuel ***,we report an integrated electrocatalyst of ultralow-Pt alloy encapsulated into nitrogen-doped nanocarbon architecture for efficient oxygen reduction *** hybrid Pt-based catalyst achieves a mass activity of 3.46 A mg^(-1)_(pt)the potential of 0.9 V *** with a negligible stability decay after 10,000 *** importantly,this half-cell activity can be expressed at full cell level with a high Pt utilization of 10.22 W mg^(-1)_(Pt cathode)and remarkable durability after 30,000 cycles in *** and theoretical investigations reveal that a highly strained Pt structure with an optimal Pt-0 binding energy is induced by the incorporation of Co/Ni into Pt lattice,which would account for the improved reaction *** synergistic catalysis due to nitrogen-doped nanocarbon architecture and active Pt component is responsible for the enhanced catalytic ***,the strong metal-support interaction and optimized hydrophilic properties of nanocarbon matrix facilitate efficient mass transport and water *** work may provide significant insights in designing the low-Pt integrated electrocatalysts for fuel cells and beyond.

摘要：Lithium-sulfur(Li-S) batteries have attracted considerable attention due to their high energy density(2600 Wh kg-1). However, its commercialization is hindered seriously by the low loading and utilization rate of sulfur cathodes. Herein, we designed the cellulose-based graphene carbon composite aerogel(CCA) self-standing electrode to enhance the performance of Li-S batteries. The CCA contributes to the mass loading and utilization efficiency of sulfur, because of its unique physical structure: low density(0.018 g cm-3), large specific surface area(657.85 m2 g-1), high porosity(96%), and remarkable electrolyte adsorption(42.25 times). Compared to Al(about 49%), the CCA displayed excellent sulfur use efficiency(86%) and could reach to high area capacity of 8.60 mAh cm-2 with 9.11 mgS loading. Meanwhile,the CCA exhibits the excellent potential for pulse sensing applications due to its flexibility and superior sensitivity to electrical response signals.