Developing effective catalysts based on earth abundant elements is critical for CO2 electroreduction. However, simultaneously achieving a high Faradaic efficiency (FE) and high current density of CO (jCO) remains a challenge. Herein, we prepare a Mn single-atom catalyst (SAC) with a Mn-N3 site embedded in graphitic carbon nitride. The prepared catalyst exhibits a 98.8% CO FE with a jCO of 14.0 mA cm−2 at a low overpotential of 0.44 V in aqueous electrolyte, outperforming all reported Mn SACs. Moreover, a higher jCO of 29.7 mA cm−2 is obtained in an ionic liquid electrolyte at 0.62 V overpotential. In situ X-ray absorption spectra and density functional theory calculations demonstrate that the remarkable performance of the catalyst is attributed to the Mn-N3 site, which facilitates the formation of the key intermediate COOH* through a lowered free energy barrier.
Carbon molecular sieve (CMS) membranes with rigid and uniform pore structures are ideal candidates for high temperature- and pressure-demanded separations, such as hydrogen purification from the steam methane reforming process. Here, we report a facile and scalable method for the fabrication of cellulose-based asymmetric carbon hollow fiber membranes (CHFMs) with ultramicropores of 3–4 Å for superior H2 separation. The membrane fabrication process does not require complex pretreatments to avoid pore collapse before the carbonization of cellulose precursors. A H2/CO2 selectivity of 83.9 at 130 °C (H2/N2 selectivity of >800, H2/CH4 selectivity of >5700) demonstrates that the membrane provides a precise cutoff to discriminate between small gas molecules (H2) and larger gas molecules. In addition, the membrane exhibits superior mixed gas separation performances combined with water vapor- and high pressure-resistant stability. The present approach for the fabrication of high-performance CMS membranes derived from cellulose precursors opens a new avenue for H2-related separations.
12 February 2021 in Energy & Environmental Science
Amino-modification, as an ingenious strategy, was proposed for boosting CO 2 electroreduction current density of Ni–N/C single-atom catalyst to industrial level.
22 January 2020 in ACS Sustainable Chemistry & Engineering