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Exploring efficient non-precious metal cathode catalysts is attracting ever-increasing interest in the development of direct borohydride fuel cell (DBFC). Herein, a cobalt-based nitrogen-doped bamboo-like graphene tube (Co-NGT) is prepared as an efficient cathode catalyst. The Co-NGT consists of bamboo-like graphene tubes (40–130 nm in diameter and ∼10 μm in length), as well as cobalt nanoparticles (50–100 nm in diameter) confined in the graphene tubes. The Co-NGT shows an onset reduction potential of 0.964 V and an almost four-electron pathway towards oxygen reduction reaction, as well as a negative shift of 8 mV in half-wave potential after 10,000 CV cycles. The Tafel slope of the Co-NGT catalyst is 47 mV decade−1, which is by ca. 37.8 mV decade−1 smaller than for Pt/C. A DBFC using the Co-NGT cathode yields the biggest power density of 453 mW cm−2 at 60 °C and a life span of over 120 h. The excellent electrocatalytic properties and superior durability of Co-NGT catalyst arise from the highly graphitized NGT, providing strong interaction with Co nanoparticles and mitigating the agglomeration of Co nanoparticles. Our study guides for composition and structural design of high-efficient cathode catalysts of DBFC. [Display omitted] • The Tafel slope of Co-NGT towards ORR is 47 mV dec−1. • The half-wave potential is only 8 mV negative shift of Co-NGT after 10,000 CV cycles. • Maximum power density of 453 mWcm−2 is achieved by DBFC using Co-NGT cathode. [ABSTRACT FROM AUTHOR]

Designing efficient and stable single-atom catalysts (SACs) for the oxygen reduction reaction (ORR) is essential to promote fuel cell commercialization. In this study, the Bayesian Regularization Neural Network (BRNN) has been used to determine the carbothermal shock (CTS) conditions for preparing high-loading Pt-Fe/C SACs. The BRNN model effectively identified a low reaction temperature of 283 °C for achieving high-loading (15 wt %) Pt-Fe/C SACs. Based on this model, we successfully synthesized Pt-Fe/C SACs with a metal mass content of 11.31 wt % using the CTS method. These ultrahigh content metal Pt-Fe/C SACs consisted of dispersed single atoms and foam-like atomic constructions, namely Pt-Fe/C atom foam catalysts (AFCs), rendered them promising candidates for electrocatalysis applications. The Pt-Fe/C AFCs exhibited good catalytic activity and durability toward ORR in alkaline conditions. The Pt-Fe/C AFCs were employed in a direct borohydride fuel cell (DBFC) as cathode catalyst, which resulted in a maximum power density of 214 mW cm−2 at 60 °C and demonstrated stable discharge for 40 h at room temperature. The electrocatalytic performance of the Pt-Fe/C AFCs surpassed that of low-loading Pt-Fe/C SACs and commercial Pt/C catalysts. The rapid ramp-up rate and the rapid cooling rate of the CTS process enabled the incorporation of high-loading Pt and Fe metal atoms into the graphitized carbon layer, resulting in an increased number of active sites of the Pt-Fe/C AFCs. This work provides an effective strategy for manufacturing efficient and stable SACs for practical applications in fuel cells. [Display omitted] • The Bayesian Regularization Neural Network is used to determine the CTS conditions. • Pt-Fe/C AFCs with metal content of 11.31 wt % is successfully synthesize by the CTS method. • The Pt-Fe/C AFCs exhibit good catalytic activity and durability towards ORR. • The DBFC using Pt-Fe/C AFCs cathode achieves a maximum power density of 214 mW cm−2. [ABSTRACT FROM AUTHOR]

Designing an efficient and stable non-precious metal cathode catalyst is essential to reduce fuel cell cost and promote fuel cell commercialization. Herein, ZIF-67 and carbon powder are rapidly heated using a transient Joule heat device to pyrolyze ZIF-67 to form a CoO/N/C nanocatalysts. The prepared CoO/N/C-90 is comprised of 3–4 nm CoO nanoparticles loaded on a carbon substrate. In alkaline medium the Tafel slope of CoO/N/C-90 is 50 mV dec−1, and a half-wave potential (E 1/2) of 0.82 V towards oxygen reduction reaction (ORR). The E 1/2 only experiences a negative shift of 4 mV after 40,000 cyclic voltammetry (CV) cycles, demonstrating excellent catalytic reaction kinetics and durability. The CoO/N/C-90 is assembled into direct borohydride fuel cells (DBFC) as a cathode, achieving a maximum power density (P max) of 526 mW cm−2 at 60 °C. This work indicates that the CoO/N/C-90 is an efficient and stable non-precious metal catalyst for DBFCs. [Display omitted] • CoO/N/C nanoparticle with a size of 3–4 nm is prepared by CTS method. • CoO/N/C exhibits superior stability and highly electrochemically active area. • A DBFC with maximum power density of 526 mW cm−2 is achieved at 60 °C. [ABSTRACT FROM AUTHOR]

• In situ XANES was used to reveal the valence evolution of Fe-based electrocatalysts toward ORR. • In situ XRD was used to reveal the phase transition of Fe-based electrocatalysts during ORR. • A Fe2+/3+ redox transition was both found in Fe-PPy-C and FeS-PPy-C. • The Fe, FeS and Fe 2 O 3 were all converted to FeOOH during ORR in Fe-based electrocatalysts. • The ORR activities of Fe-based electrocatalysts are governed by their static structure. [Display omitted] The commercialization of fuel cells relies largely upon the development of highly active non-precious metal electrocatalysts. Insufficient understanding of the reaction mechanism of Fe-based electrocatalysts towards oxygen reduction reaction (ORR) limits the further improving of its catalytic performance. Herein the valence state and phase transformation of three Fe-based electrocatalysts comprising different valences of iron during the ORR in alkaline medium are investigated by in situ synchrotron radiation X-ray absorption and diffraction studies in direct borohydride fuel cell. There is a dynamic structure associated with the 'Fe2+/3+' redox transition confirmed by in situ X-ray absorption near edge structure spectra in Fe-PPy-C and FeS-PPy-C. The metallic Fe, FeS, and Fe 2 O 3 of the three Fe-based electrocatalysts are all converted to FeOOH during ORR. The local structure of Fe atoms and valence transition barrier contribute to most of the ORR activities of the three Fe-based electrocatalysts. [ABSTRACT FROM AUTHOR]