Metal-organic frameworks (MOFs) are a class of promising materials for diverse heterogeneous catalysis, but they are usually not directly employed for oxygen evolution electrocatalysis. Most reports focus on using MOFs as templates to in situ create efficient electrocatalysts through annealing. Herein, we prepared a series of Fe/Ni-based trimetallic MOFs (Fe/Ni/Co(Mn)-MIL-53 accordingly to the Material of Institute Lavoisier) by solvothermal synthesis, which can be directly adopted as highly efficient electrocatalysts. The Fe/Ni/Co(Mn)-MIL-53 shows a volcano-type oxygen evolution reaction (OER) activity as a function of compositions. The optimized Fe/Ni /Co -MIL-53 can reach a current density of 20 mA cm at low overpotential of 236 mV with a small Tafel slope of 52.2 mV dec . In addition, the OER performance of these MOFs can be further enhanced by directly being grown on nickel foam (NF).
Pursuing active and durable water splitting electrocatalysts is of vital significance for solving the sluggish kinetics of the oxygen evolution reaction (OER) process in energy supply. Herein, theoretical calculations identify that the local distortion-strain effect in amorphous RuTe2 system abnormally sensitizes the Te-pπ coupling capability and enhances the electron-transfer of Ru-sites, in which the excellent inter-orbital p-d transfers determine strong electronic activities for boosting OER performance. Thus, a robust electrocatalyst based on amorphous RuTe2 porous nanorods (PNRs) is successfully fabricated. In the acidic water splitting, a-RuTe2 PNRs exhibit a superior performance, which only require a cell voltage of 1.52 V to reach a current density of 10 mA cm−2. Detailed investigations show that the high density of defects combine with oxygen atoms to form RuOxHy species, which are conducive to the OER. This work offers valuable insights for constructing robust electrocatalysts based on theoretical calculations guided by rational design and amorphous materials.
Carbon dioxide (CO2) hydrogenation
to ethanol (C2H5OH) is considered a promising
way for CO2 conversion and utilization, whereas desirable
conversion
efficiency remains a challenge. Herein, highly active, selective and
stable CO2 hydrogenation to C2H5OH
was enabled by highly ordered Pd-Cu nanoparticles (NPs). By tuning
the composition of the Pd-Cu NPs and catalyst supports, the efficiency
of CO2 hydrogenation to C2H5OH was
well optimized with Pd2Cu NPs/P25 exhibiting high selectivity
to C2H5OH of up to 92.0% and the highest turnover
frequency of 359.0 h–1. Diffuse reflectance infrared
Fourier transform spectroscopy results revealed the high C2H5OH production and selectivity of Pd2Cu NPs/P25
can be ascribed to boosting *CO (adsorption CO) hydrogenation to *HCO,
the rate-determining step for the CO2 hydrogenation to
C2H5OH.
The renewable electricity-driven reduction of carbon dioxide (CO 2 RR) is a promising technology for carbon utilization. However, it is still a challenge to broaden the application of CO 2 RR. Herein, we report a Te-doped Pd nanocrystals (Te−Pd NCs) for promoting urea synthesis by coupling CO 2 RR with electrochemical reduction of nitrite. The electrochemical synthesis of urea has been achieved with nearly 12.2% Faraday efficiency (FE) and 88.7% N atom efficiency (NE) at −1.1 V versus reversible hydrogen electrode (vs RHE), much higher than those of pure Pd NCs (4.2% FE and 21.8% NE). Significantly, an FE of ∼10.2% and an NE of ∼82.3% for urea solution production via an optimized flow cell system have been realized, where a solution with up to 0.95 wt % of urea has been obtained. Mechanistic insights show that Te-doping not only optimizes the CO 2 / CO adsorption but also promotes NH 3 production, fully meeting the requirements of urea synthesis.
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