As a fascinating two-dimensional (2D) conjugated polymer, graphitic carbon nitride (C 3 N 4 ) has drawn broad attention as metal-free photocatalyst, but it’s further utilization is confined by the limited visible light harvesting and severe charge recombination. Herein, N-rich carbon nitride (C 3 N 5 ) with an azo-linked two s -heptazine units, different from C 3 N 4 with a tertiary N-atom linked three s -heptazines, is prepared for constructing a novel sandwich heterojunction composed of reduced graphene oxide (rGO)-coupled C 3 N 5 and C 3 N 4 . The introduced rGO in C 3 N 4 /rGO/C 3 N 5 heterojunction can accelerate the interfacial charge separation and promote a rGO-mediated solid-state Z-scheme mechanism with an obvious synergistic effect, whereby C 3 N 4 and C 3 N 5 serve as electron-rich and hole-rich reservoirs, respectively. The resultant 2D/2D heterojunction delivers efficient visible-light-responsive activity with H 2 evolution rate of 319 μmol h -1 , 5.6 and 2.7 times higher than that of C 3 N 4 and C 3 N 5 alone, respectively. This work presents a new concept to design highly efficient carbon nitride-based artificial photosynthetic system. • rGO-coupled C 3 N 4 /C 3 N 5 2D/2D Z-scheme heterojunction is prepared for the first time • Significantly retarded charge recombination promotes fascinating H 2 evolution activity • Metal-labelled experiments confirm the sandwich structure of the 2D/2D heterojunction • A Z-scheme mechanism was proved using (photo)electrochemical and in-situ CPD techniques 

Construction of rGO-coupled C3N4/C3N5 2D/2D Z-scheme heterojunction to accelerate charge separation for efficient visible light H2 evolution

Synthesis of oriented J type ZnIn2S4@CdIn2S4 heterojunction by controllable cation exchange for enhancing photocatalytic hydrogen evolution.

Pre-intercalation of phosphate into Ni(OH)2/NiOOH for efficient and stable electrocatalytic oxygen evolution reaction

With photovoltaics becoming a mature, commercially feasible technology, society is willing to allocate resources for developing and deploying new technologies based on using solar light. Analysis of projects supported by the European Commission in the past decade indicates exponential growth of funding to photocatalytic (PC) and photoelectrocatalytic (PEC) technologies that aim either at technology readiness levels (TRLs) TRL 1–3 or TRL > 3, with more than 75 Mio€ allocated from the year 2019 onward. This review provides a summary of PC and PEC processes for the synthesis of bulk commodities such as solvents and fuels, as well as chemicals for niche applications. An overview of photoreactors for photocatalysis on a larger scale is provided. The review rounds off with the summary of reactions performed at lab scale under natural outdoor solar light to illustrate conceptual opportunities offered by solar-driven chemistry beyond the reduction of CO2 and water splitting. The authors offer their vision of the impact of this area of research on society and the economy.

Progress in Development of Photocatalytic Processes for Synthesis of Fuels and Organic Compounds under Outdoor Solar Light

Hydrogen production through electrochemical water splitting (EWS) presents a viable solution for addressing the fossil energy crisis. However, the commercial viability of this approach is impeded by the sluggish kinetics of the oxygen evolution reaction (OER). It is urgently needed to develop efficient, stable, and cost-effective OER electrocatalysts. Herein, we comprehensively design and investigate a phosphate ion and Fe3+ codecorating Ni(OH)2/NiOOH electrocatalyst (Pi-Fe:NiOH) for OER. This codecoration induces multiple synergistic effects, which include an increase in the interlayer water content for the internal OER, altering the OER mechanism, facilitating proton transport across the layers, and improving the stability of Pi-Fe:NiOH. Consequently, Pi-Fe:NiOH exhibits a high OER activity with overpotentials of 118 ± 1 and 222 ± 4 mV at current densities of 10 and 100 mA cm–2, respectively. More impressively, it maintains stable operation at a high current density of around 300 mA cm–2 for at least 500 h, much better than the Ni(OH)2/NiOOH electrocatalyst (NiOH) for less than 6 h at a current density below 200 mA cm–2. These findings offer insights for the design of anion–cation codoped hydroxide eletrocatalysts, paving a way for the development of efficient and stable OER electrocatalysts. 

Codecoration of Phosphate and Iron for Improving Oxygen Evolution Reaction of Layered Ni(OH)2/NiOOH

Hierarchically Porous Polymeric Carbon Nitride as a Volume Photocatalyst for Efficient H2 Generation under Strong Irradiation

Volume Photocatalysis In article number 2100823, Yuexiang Li and co-workers found that tube-like polymeric carbon nitride with wall nanopores which was prepared by pyrolyzing needle-like urea, shows enhanced photoabsorption under strong irradiation, and allows the reactant formic acid to effectively insert into its volume/interlayers. Different from conventional surface photocatalysis, the reaction efficiency of the volume photocatalysis rises with irradiation intensity. 

Hierarchically Porous Polymeric Carbon Nitride as a Volume Photocatalyst for Efficient H
 2
 Generation under Strong Irradiation

A nonstoichiometric La1.5Sr0.5Ga3O7.25 melilite oxide ion conductor features active interstitial oxygen defects in its pentagonal rings with high mobility. In this study, electron localization function calculated by density functional theory indicated that the interstitial oxide ions located in the pentagonal rings of gallate melilites may be removed and replaced by electron anions that are confined within the pentagonal rings, which would therefore convert the melilite interstitial oxide ion conductor into a zero-dimensional (0D) electride. The more active interstitial oxide ions, compared to the framework oxide ions, make the La1.5Sr0.5Ga3O7.25 melilite structure more reducible by CaH2 using topotactic reduction, in contrast to the hardly reducible nature of parent LaSrGa3O7. The topotactic reduction enhances the bulk electronic conduction (σ ∼ 0.003 S/cm at 400 °C) by ∼ 1 order of magnitude for La1.5Sr0.5Ga3O7.25. The oxygen loss in the melilite structure was verified and most likely took place on the active interstitial oxide ions. The identified confinement space for electronic anions in melilite interstitial oxide ion conductors presented here provides a strategy to access inorganic electrides from interstitial oxide ion conductor electrolytes.

Theoretical and Experimental Studies of Gallate Melilite Electrides from Topotactic Reduction of Interstitial Oxide Ion Conductors.

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Synthesis of oriented J type ZnIn2S4@CdIn2S4 heterojunction by controllable cation exchange for enhancing photocatalytic hydrogen evolution.

Hierarchically Porous Polymeric Carbon Nitride as a Volume Photocatalyst for Efficient H2 Generation under Strong Irradiation

Hierarchically Porous Polymeric Carbon Nitride as a Volume Photocatalyst for Efficient H 2 Generation under Strong Irradiation

Theoretical and Experimental Studies of Gallate Melilite Electrides from Topotactic Reduction of Interstitial Oxide Ion Conductors.