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Biochar-assisted water electrolysis (BAWE) facilitates the high-value utilization of biomass and energy-saving hydrogen production. However, the BAWE efficiency is hindered by slow kinetics of biochar oxidation reaction (BOR) at anode. Herein, to improve the overall efficiency of BAWE, three-dimensional porous nanosheets modified on nickel foam (Ni 1 Fe 2 -LDH@NF) was developed for BOR, and its mechanism was identified. Impressively, the BAWE system exhibited remarkable activity, including a low potential of 1.387 V vs. RHE for BOR over as-synthesized electrocatalyst at current density of 10 mA·cm−2, and excellent long-term stability over 20 h at a high current density of 200 mA·cm−2 and after 1000 CV cycles. The required electricity input was 3.29 kWh·Nm−3H 2 at 10 mA·cm−2 for BAWE with Ni 1 Fe 2 -LDH@NF toward BOR. In addition, the reaction mechanism of BOR including biochar direct oxidation on the electrocatalysts surface and indirect oxidation in the electrolyte was deduced, according to the surface chemistry and composition changes of electrocatalysts and biochar, as well as the products. This work provides an effective strategy towards the enhancement of the BOR process by designing the binder-free electrocatalysts, and facilitates the development of BAWE for energy-efficient hydrogen production and biomass utilization. [Display omitted] • 3D porous Ni–Fe nanosheets modified on nickel foam was developed for enhancing BOR. • Ni 1 Fe 2 -LDH@NF favored the adsorption of OH− and accelerated the charge transfer rate. • Ni 1 Fe 2 -LDH@NF toward BOR demonstrated a potential of 1.387 V vs. RHE@10 mA·cm−2 and stability over 20 h@200 mA·cm−2. • The BOR mechanism including biochar direct oxidation on electrocatalysts and indirect oxidation in electrolyte was deduced. [ABSTRACT FROM AUTHOR]

Highly-efficient and stable non-noble metal electrocatalysts for overcoming the sluggish kinetics of oxygen evolution reaction (OER) is urgent for water electrolysis. Biomass-derived biochar has been considered as promising carbon material because of its advantages such as low-cost, renewable, simple preparation, rich structure, and easy to obtain heteroatom by in-situ doping. Herein, Ni 2 P–Fe 2 P bimetallic phosphide spherical nanocages encapsulated in N/P-doped pine needles biochar is prepared via a simple two-step pyrolysis method. Benefiting from the maximum synergistic effects of bimetallic phosphide and biochar, high conductivity of biochar encapsulation, highly exposed active sites of Ni 2 P–Fe 2 P spherical nanocages, rapid mass transfer in porous channels with large specific surface area, and the promotion in adsorption of reaction intermediates by high-level heteroatom doping, the (Ni 0.75 Fe 0.25) 2 P@NP/C demonstrates excellent OER activity with an overpotential of 250 mV and a Tafel slope of 48 mV/dec at 10 mA/cm2 in 1 M KOH. Also it exhibits a long-term durability in 10 h electrolysis and its activity even improves during the electrocatalytic process. The present work provides a favorable strategy for the inexpensive synthesis of biochar-based transition metal electrocatalysts toward OER, and improves the water electrolysis for hydrogen production. [Display omitted] • Ni 2 P–Fe 2 P spherical nanocages encapsulated in N/P-doped biochar is synthesized. • High-level heteroatom ((N + P + O): C) doping of 30.61 at% is achieved. • OER over (Ni 0.75 Fe 0.25) 2 P@NP/C demonstrates an overpotential of 250 mV@10 mA/cm2. • The synergistic effect of Ni 2 P–Fe 2 P and N/P-doped biochar promotes OER. [ABSTRACT FROM AUTHOR]

A novel sulfur–iodine (SI or IS) cycle integrated with HI–I 2 –H 2 O electrolysis for hydrogen production was developed and thermodynamically analyzed in this work. HI–I 2 –H 2 O electrolysis was used to replace the conventional concentration, distillation, and decomposition processes of HI, so as to simplify the flowsheet of SI cycle. And then the new cycle was divided into Bunsen reaction, H 2 SO 4 decomposition and HI–I 2 –H 2 O electrolysis sections. Through incorporating the user-defined module of HI–I 2 –H 2 O electrolysis with Aspen Plus, the cycle was simulated and 0.448 mol/h (10 L/h) of H 2 was produced. The overall energy and exergy efficiencies of the novel SI system were estimated to be 15.3–31.0% and 32.8%, respectively. Most exergy destruction occurred in the H 2 SO 4 decomposer and condenser for H 2 SO 4 decomposition and Bunsen reaction sections, which accounted for 93.0% and 63.4%, respectively. A high exergy efficiency of 92.4% for HI–I 2 –H 2 O electrolysis section with less exergy destruction was determined, mostly due to the transformation of the overall electricity in electrolytic cell to exergy. Appropriate internal heat exchange and waste heat recovery will favor improving the energy and exergy efficiencies. • A new SI cycle assembled with HI–I 2 –H 2 O electrolysis was thermodynamically analyzed. • Exergy destruction and exergy efficiency for each section were evaluated. • A high exergy efficiency of 92.4% for HI–I 2 –H 2 O electrolysis section was found. • The energy and exergy efficiencies of 15.3–31.0% and 32.8% were estimated for SI cycle. [ABSTRACT FROM AUTHOR]