The synthesis of multi-carbon (C2+) fuels via electrocatalytic reduction of CO, H2O using renewable electricity, represents a significant stride in sustainable energy storage and carbon recycling. The foremost challenge in this field is the production of extended-chain carbon compounds (Cn, n ≥ 3), wherein elevated *CO coverage (θco) and its subsequent multiple-step coupling are both critical. Notwithstanding, there exists a “seesaw” dynamic between intensifying *CO adsorption to augment θco and surmounting the C-C coupling barrier, which have not been simultaneously realized within a singular catalyst yet. Here, we introduce a facilely synthesized lattice-strain-stabilized nitrogen-doped Cu (LSN-Cu) with abundant defect sites and robust nitrogen integration. The low-coordination sites enhance θco and concurrently, the compressive strain substantially fortifies nitrogen dopants on the catalyst surface, promoting C-C coupling activity. The n-propanol formation on the LSN-Cu electrode exhibits a 54% faradaic efficiency and a 29% half-cell energy efficiency. Moreover, within a membrane electrode assembly setup, a stable n-propanol electrosynthesis over 180 h at a total current density of 300 mA cm−2 is obtained.
Sodium borohydride (NaBH4) is a nontoxic and ideal storage material for hydrogen due to its safety and high hydrogen storage capacity. In order to improve the practicality of the sodium borohydride hydrogen production system, we deposited non-precious metal catalytic materials on readily available polymer foams using a simple chemical plating method, developing a suitable 3D catalyst. Its high specific surface area enables it to produce hydrogen at a rate of up to 3.92 L min−1 g−1. Its unique structure gives the catalyst excellent durability. In addition, an efficient NaBH4-based H2 supply system was developed using this catalyst. Co-Cu-B can facilitate stable hydrogen production from NaBH4, yielding a consistent power output ranging from 0 to 100 W. This work provides a new pathway for developing high-efficiency monolithic self-supported catalysts for industrial applications.
Dimethylamine borane (DMAB) is a promising solid fuel for borane fuel cells due to its high hydrogen content and safety. However, the development is hindered by electrochemically sluggish DMAB oxidation reaction (DMABOR), since strongly adsorbed hydrogen‐containing reaction intermediates (*H) poison active sites. Herein, a Mo‐single‐atom‐enabled functional‐site‐decoupled PdMo catalyst is developed by combining functional‐site decoupling with atomic‐level oxophilic engineering. Spectroscopy and theoretical studies reveal that the catalyst comprises PdMo alloy particles (APs) and Mo single atoms (SAs), wherein alloyed Mo modulates electronic structure of Pd to weaken *H binding, and Mo SAs act as *OH‐affinitive Lewis‐acid sites that stabilize interfacial *OH, which is proposed to assist the oxidative removal of Pd‐bound *H. Notably, PdMo/KB was applied as the anode in direct DMAB fuel cells (D‐DMABFCs) for the first time, enabling an outstanding peak power density of 1195 mW cm −2 and stable operation for over 160 h, highlighting the potential of borane fuel cells as alternatives to hydrogen fuel cells. This functional‐site‐decoupling mechanism is further extended to alkaline hydrogen evolution reaction (HER), enabling a PdMo/KB‐based anion‐exchange membrane water electrolyzer (AEMWE) to reach 1.0 and 2.0 A cm −2 at 1.59 and 1.70 V, respectively, and operate stably for 1000 h.
An electrochemical reduction of CO2 to CO has become a challenging issue in CO2 utilization in order to mitigate the climate change. In this study, we report a promising approach to prepare Au-based electrocatalysts for the electrochemical reduction of CO2 to CO having the maximized activity/selectivity and the minimized Au usage. It was clearly confirmed that the Au thin layer formed by the electrochemical galvanic displacement on polycrystalline Cu surface resulted in a markedly enhanced performance for the electrochemical reduction of CO2 to CO. The CO Faradaic efficiency for the Au thin layer on Cu was 10.6 and 3.4 times higher than that for the polycrystalline Cu and Au, respectively. It was revealed from the photoemission spectroscopy (PES) studies that the increase of electron population in s-band and the upshift of d-band center position of Au in Au/Cu increased the bond strength with reaction intermediates leading to the enhancement of activity and the selectivity. Along with the electronic effect, the geometric effect like the increased the electrochemical surface area (ECSA) and proportion of low coordinated sites also played a substantial role in the performance enhancement.
High‐temperature proton exchange membrane water electrolysis (HT‐PEMWE) is a promising strategy for low‐energy, high‐efficiency hydrogen production. However, practical implementation relies critically on the development of novel PEMs that simultaneously offer high proton conductivity and long‐term stability at high temperatures. While metal–organic frameworks (MOFs) have been widely investigated as high‐performance proton‐conducting materials, their specific incorporation into Nafion matrices for HT‐PEMWE remains largely unexplored. In this work, we designed and fabricated a sulfonated MOF‐reinforced Nafion (S/N‐Nafion) composite membrane. The S/N‐Nafion membrane achieved a proton conductivity of 154.7 mS cm −1 at 100 °C, which is twice that of recast Nafion (75.6 mS cm −1 ), while also possessing excellent mechanical strength and dimensional stability at elevated temperatures. When used as the solid electrolyte, an electrolyzer with S/N‐Nafion reached only 1.59 V at 120 °C and 3.0 A cm −2 , which is 120 mV lower than recast Nafion (1.71 V) under the identical conditions. Moreover, during a 300‐h durability test at 120 °C and 1.0 A cm −2 , the S/N‐Nafion‐PEMWE exhibited an extremely low voltage decay rate of 6.0 µV h −1 . These results underscore the immense potential of the S/N‐Nafion membrane for enabling highly efficient and stable high‐temperature electrolytic hydrogen production.