Wendan Nie,Yixing Luo,Qifeng Yang,Gang Feng,Qilu Yao,Zhang-Hui Lu
Selective dehydrogenation of formic acid (FA, HCOOH) is a promising alternative to fossil fuels, to provide a clean energy carrier for the future energy economy. The preparation of highly efficient catalysts for hydrogen release from FA at room temperature has attracted much attention but still remains a great challenge. Herein, ultrafine bimetallic PdIr nanoparticles (NPs) immobilized by amine-functionalized SBA-15 (PdIr/SBA-15-NH2) have been successfully synthesized via a facile surface functionalization and co-reduction method. The characterized results showed that ultrafine bimetallic PdIr NPs with a small size of around 1.1 nm were highly dispersed on SBA-15-NH2. Among all the as-synthesized catalysts, the optimized Pd0.85Ir0.15/SBA-15-NH2 nanocomposites (NCs) exhibited the highest catalytic activity and 100% H2 selectivity toward the selective dehydrogenation of FA, giving an initial turnover frequency (TOF) value as high as 3087 h−1 at room temperature. To the best of our knowledge, this is the first report showing that the Ir-containing heterogeneous catalyst can achieve a complete dehydrogenation of FA to H2. The excellent catalytic performance of this catalyst might be attributed to the modified electronic effects of Pd with Ir, the ultrafine size and high dispersion of PdIr NPs, and the synergetic interaction between the PdIr NPs and SBA-15-NH2. The amine functional groups of SBA-15-NH2 not only can lead to ultrafine and well-dispersed PdIr NPs and stabilize the PdIr NPs, but also can serve as Brønsted basic sites, which facilitates the O–H bond dissociation of FA and forms a formate intermediate. The present PdIr/SBA-15-NH2 NCs with efficient catalytic effects on the dehydrogenation of FA may greatly promote the practical application of the FA system on fuel cells.
Hydrogen production by biomass electrolysis offers a promising and sustainable route for producing green hydrogen and high-value utilization of biomass. However, this process consumes electricity and suffers from low anode Faraday efficiency of the organic electro-oxidation reaction. Herein, we develop a novel strategy that integrates a room-temperature, high-power lignin-derived aldehyde flow fuel cell (FFC) with hydrogen production, which converts the power-consuming electrocatalytic hydrogen production step into an electricity-generating process. The highly active Ag-Cu x O/CF (copper foam) electrocatalyst exhibits dual functionality of efficient electricity generation and simultaneous hydrogen production by catalyzing low-potential aldehyde group oxidation at the anode, which concurrently releases electrons and generates hydrogen. The Ag-Cu x O/CF electrocatalyst can significantly improve the electron transfer rate and catalytic conversion efficiency of the anode, attributable to its mixed Cu 0 /Cu + valence states, enlarged double-layer capacitance (C dl ), reduced interfacial resistance, and optimized adsorption capacity. The Ag-Cu x O/CF catalyst achieves ∼95 % benzaldehyde conversion and ∼98.4 % Faradaic efficiency for hydrogen production at 0.35 V RHE . Furthermore, the FFC based on Ag-Cu x O/CF electrocatalyst demonstrated excellent dual-functionality at room temperature, achieving both a power density of 173.5 mW cm −2 and a hydrogen production rate of 1.96 mmol cm −2 h −1 . The constructed FFC achieved a room-temperature power density threefold greater than the reported lignin-based power generation technology, while maintaining comparable hydrogen production rate to biomass electrolysis processes. This study provides a novel approach to reduce the cost of green hydrogen production and mitigate the global energy crisis.
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