Ruibin Jiang

A bifunctional electrocatalyst consisting of NiFe metal–organic framework (NiFe-MOF) grown on carbon black with FeN ₄ single sites is reported for ORR and OER in rechargeable zinc–air batteries.

Product selectivity in the electrochemical CO ₂ reduction reaction is strongly governed by the surface adsorption properties of reactant molecules and reaction intermediates. Using oxide‐derived copper as a model electrocatalyst, it is demonstrated that sulfur modification can redirect the CO ₂ reduction pathway from multicarbon products to formate by tuning the adsorption configuration of CO ₂ . Notably, this selectivity transition is highly sensitive to the concentration of sulfide ions (S ²⁻ ), with a pronounced influence even at a concentration as low as 1 μmol/L. By combining in‐situ spectroscopy characterizations, theoretical calculations of adsorbed CO ₂ reduction intermediates, and controlled CO electrolysis experiments, it is revealed that the introduction of S ²⁻ alters the adsorption mode of CO ₂ on the Cu surface from C‐site adsorption to O‐site adsorption, thus enabling the observed switch in product selectivity of CO ₂ reduction. This work provides a new perspective for understanding and steering the product selectivity of the electrochemical CO ₂ reduction reaction by engineering the adsorption configuration of key intermediates.

A synergistic structure-directing strategy to construct a Cu-TCPP NSs/Ti ₃ C ₂ T _x NSs fiber supercapacitor with good energy density and high flexibility was undertaken.

Photocatalytic urea synthesis from N2 and CO2 offers a sustainable alternative to the energy-intensive industrial process. However, the efficiency remains hindered by the sluggish C–N coupling kinetics. Herein, a new, kinetically favorable urea synthesis pathway is achieved by a rationally designed RuCu alloy/plasmonic WO3–x hybrid photocatalyst. A remarkable urea production rate of 750 μg gcat–1 h–1 together with a solar-to-chemical conversion efficiency of 0.072% is obtained under simulated sunlight illumination, outperforming those of most reported systems. Unlike commonly studied C–N coupling involving *CO and *N2, a new mechanism is proposed. This mechanism activates and reduces N2 and CO2 into the *NH2NH2 and *CO, respectively, followed by two successive C–N coupling processes to form urea with substantially reduced kinetic barriers. The RuCu alloy demonstrates a much lower energy barrier compared to pure metals, which is attributed to its optimized electronic structure and enhanced intermediate adsorption properties enabled by the intersite synergistic effect within the alloy.

Photocatalytic efficiency for H2O2 production on graphitic carbon nitride (g-C3N4) is limited by the relatively low separation efficiency of photocarriers and the sluggish kinetics of the consumption of photogenerated holes. Herein, g-C3N4 with carbon vacancies (Cv-CN) is prepared for photocatalytic H2O2 production coupled with benzyl alcohol (BzOH) oxidation. The carbon vacancies reduce the exciton binding energy, thus increasing the separation and transfer of photocarriers. The coupled BzOH oxidation accelerates the kinetics of consumption of photogenerated holes. The H2O2 production rate on Cv-CN is enhanced to approximately five times that of g-C3N4 without carbon vacancies. Meanwhile, BzOH is oxidized to benzaldehyde and benzoic acid, with selectivities of 60.1% and 32.0%, respectively. It is found that H2O2 is produced by the reduction of O2 by the photogenerated electrons through •O2– and •OOH intermediates. BzOH is oxidized to benzaldehyde mainly by photogenerated holes, but the further oxidation of benzaldehyde to benzoic acid is contributed by photogenerated holes and reactive oxygen species. Our findings not only demonstrate the photocatalytic H2O2 production coupled with value-added chemical synthesis but also deepen the understanding of the function of carbon vacancies in g-C3N4 for photocatalysis.

(Ti _1/3 V _2/3 ) ₂ CT _x have been synthesized through the etching of bimetallic MAX phase. The obtained (Ti _1/3 V _2/3 ) ₂ CT _x @S cathode exhibit the best electrochemical performance due to the optimized tuning of d-band center for both Ti and V.

Solar-driven CO2 conversion via photovoltaic-powered electrolysis offers a sustainable route for carbon utilization and renewable energy storage, yet its current output is still constrained by the low-value yield of the anodic reaction. Herein, we rationally designed a solar-compatible paired electrolysis system by coupling cathodic CO2 reduction reaction (CO2RR) with anodic off-field H2S oxidation reaction (OFSOR) mediated by the I3−/I− redox couple, enabling synchronous production of high-value formate and elemental sulfur with significantly reduced energy input. An acid-tolerant Bi-based metal−organic framework (Bi-MOF) precursor was fabricated and underwent in situ structural reconstruction to form Bi2O2CO3 as an active phase for CO2RR with a formate faradaic efficiency (FE) exceeding 90% over a wide current density range. In situ Raman spectroscopy confirmed the formation of key *HCOO− intermediates over the Bi2O2CO3, accounting for the superior formate selectivity. By coupling with the carbon cloth anode, a two-electrode CO2RR-OFSOR electrolyzer was assembled, delivering a current density of 50 mA/cm2 at a cell voltage of only 2.91 V and reducing cell voltage by 41% under the tested conditions as compared to the conventional CO2RR-OER configuration. Furthermore, a self-driven solar-powered photovoltaic-electrochemical device was established by directly powering the electrolyzer with commercial silicon photovoltaic cells, which steadily operates with formate FE above 90% and achieves a solar-to-chemical conversion efficiency of 4.6%. This work provides a promising and energy-efficient solar-driven integrated strategy for collaborative CO2 conversion and H2S resource utilization, highlighting the potential of hybrid electrolysis systems in sustainable electrosynthesis.

Photo-assisted Li–gas batteries have been recognized as one of the most effective strategies for reducing charge/discharge overpotential by incorporating photoelectrodes into conventional gas cathodes. However, the current photo-electrodes have still faced several issues, including narrow solar absorption, inadequate charge carrier separation, etc., which seriously restricted their rate capability and application in complicated Li–Air batteries. Herein, a series of the functionalized D–A configuration COF-n compounds with tunable built-in electric field and low charge-carrier recombination rates were designed and synthesized by optimizing the intramolecular electron distribution. The optimized benzoquinone-based COF-2 exhibited the lowest transition barrier of photon-generated carriers for impressive light absorption, exciton dissociation and charge separation, meanwhile its large D–A potential difference constructed ultra-strong electron push–pull effect, resulting in the strongest and even-distributed built-in electric field. Therefore, the assembled COF-2 based photo-assisted Li–Air battery delivered a record round-trip efficiency of 98% with discharge potential up to 3.34 V at 200 mA g⁻¹. Remarkably, the battery maintained prominent rate capability with a round-trip efficiency of 72% even at a high current density of 1000 mA g⁻¹, demonstrating reversible conversion of Li₂O₂, Li₂CO₃ and Li₃N. These findings highlight the significance of ultra-strong electron push–pull effect and low transition barrier in photo-assisted Li–Air batteries.

IrO ₂ as the most stable electrocatalyst for acidic oxygen evolution reaction (OER) suffers from its low activity and the limited abundance in earth crust. Doping is one of promising strategies to enhance the OER activity and stability of IrO ₂ . Herein, an interstitial carbon‐doped IrO ₂ (C _in ‐IrO ₂ ) catalyst is prepared for acidic OER. The C _in ‐IrO ₂ shows an OER overpotential of 227 mV at 10 mA cm ⁻² , a mass activity of 565.1 A g _Ir ⁻¹ at 1.53 V, and a 2000‐h stability with a degradation rate of 0.04 mV h ⁻¹ . The enhanced OER activity and stability originate from the formation of C─Ir bonds in the C _in ‐IrO ₂ , which results in a prominent down‐shift of Ir d ‐band center and the up‐shift of O p ‐band center. Such variations of electronic states not only optimize the adsorption of OER intermediates but also increases the covalence of Ir─O bond. The C _in ‐IrO ₂ also enables an intra‐surface hydrogen abstraction from *OOH to produce *OO, which also enhances the OER activity. The C _in ‐IrO ₂ ‐based proton exchange membrane (PEM) water electrolyzer delivers a ultrasmall cell voltages of 1.51 V at 1 A cm ⁻² and 1.96 V at 3 A cm ⁻² . Our findings demonstrate a new method for enhancing the acidic OER performance of IrO ₂ .