CO2 electrochemical reduction (CO2RR) can mitigate environmental issues while providing valuable products, yet challenging in activity, selectivity, and stability. Here, a CuS‐Bi2S3 heterojunction precursor is reported that can in situ reconstruct to Cu‐doped Bismuth (CDB) electrocatalyst during CO2RR. The CDB exhibits an industrial‐compatible current density of −1.1 A cm−2 and a record‐high formate formation rate of 21.0 mmol h−1 cm−2 at −0.86 V versus the reversible hydrogen electrode toward CO2RR to formate, dramatically outperforming currently reported catalysts. Importantly, the ultrawide potential region of 1050 mV with high formate Faradaic efficiency of over 90% and superior long‐term stability for more than 100 h at −400 mA cm−2 can also be realized. Experimental and theoretical studies reveal that the remarkable CO2RR performance of CDB results from the doping effect of Cu which optimizes adsorption of the *OCHO and boosts the structural stability of metallic bismuth catalyst. This study provides valuable inspiration for the design of element‐doping electrocatalysts to enhance catalytic activity and durability.
The intrinsic sluggish kinetics of the oxygen evolution reaction (OER) limit the improvement of hydrogen evolution reaction (HER) performance, and substituting the anodic oxidation of biomass materials is an alternative approach, given its lower oxidation potential and higher added value compared to those of OER. In this study, a Ni3S2‐MoS2 nanoheterojunction catalyst with strong electronic interactions is prepared. It exhibits high efficiency for both the HER and the electrooxidation of 5‐hydroxymethylfurfural (HMF). In a two‐electrode cell with Ni3S2‐MoS2 serving as both the anode and cathode, the potential is only 1.44 V at a current density of 10 mA cm−2, which is much lower than that of pure water splitting. Density functional theory calculations confirm that the strong chemisorption of H and HMF at the interface leads to outstanding electrocatalytic activity. The findings not only provide a strategy for developing efficient electrocatalysts, but also provide an approach for the continuous production of high value‐added products and H2.
Ni-loaded CeO 2 -based materials are one type of the promising catalyst for CO 2 methanation; however, lowering the Ni loading, simplifying the preparation process of CeO 2 supports, and improving the low-temperature catalytic performance are always essential for scalable applications. Herein, an efficient CeO 2 support (CeO 2 -NC) with a large inner pore size was prepared by a facilely controlled calcination of cerium nitrate [Ce(NO 3 ) 3 •6H 2 O] method. On the basis of CeO 2 -NC, one catalyst (Ni/CeO 2 -NC) with low Ni loading (2.56 wt %), desirable Ni dispersity, and abundant medium basic sites was developed that exhibited the amazing low-temperature CO 2 methanation performance. At 275 °C, CO 2 conversion reached up to 77.7% with an almost 100% CH 4 selectivity under a high gas hourly space velocity of 60000 mL g cat −1 h −1 , and the Ni-based mass-specific CH 4 formation rate at 300 °C was up to 4740 μmol g Ni −1 s −1 , outperforming most of the reported Ni-based catalysts to date. The in situ diffuse-reflectance infrared Fourier transform spectroscopy experiments revealed that plentiful active bidentate carbonate intermediates and effective suppression of the dissociated active H species recombination contributed to the boosted CO 2 methanation performance of Ni/CeO 2 -NC at low temperatures. Moreover, the mechanism was also inferred. This work provides new insight into simple pyrolysis CeO 2 supports and should be of significance for the rational design of highly efficient CO 2 methanation catalysts.
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