The development of advanced technology for producing high‐purity and low‐cost hydrogen is crucial for the upcoming hydrogen economy. One of the most promising technologies to achieve carbon peak and carbon neutrality is hydrogen production through water electrolysis coupled with renewable energy. However, the efficiency of water electrolysis is limited by the catalyst material employed, thereby the pursuit of highly efficient catalysts is of paramount scientific significance. In this review, we focus on the synthesis of electrocatalysts for the hydrogen/oxygen evolution reaction (HER/OER) through various strategies such as hydrogen spillover, heterostructure construction, element doping, monatomic construction, LDH structure modification, high entropy alloy, and other approaches. The article also provides a comprehensive overview of the challenges encountered in enhancing the activity, stability, and durability of transition metal heterogeneous catalysts for both HER and OER. Moreover, the mechanisms of HER and OER are illustrated. The electrocatalysts prepared by these strategies have exhibited promising results in terms of water splitting performance. However, there are still unresolved issues that need to be addressed, such as improving long‐term stability and reducing overall cost. Future prospects include exploring new materials and optimizing the preparation methods to further enhance the electrocatalytic activity.

Recent advances and perspective on transition metal heterogeneous catalysts for efficient electrochemical water splitting

The photocatalysis conversion of CO2 into fuels has become an encouraging method to address climate and energy issues as a long-term solution. Single material suffers poor yield due to low light energy utilization and high recombination rate of photoinduced electron-hole pairs. It is an efficient approach to construct heterojunction through two or three materials to improve the photocatalytic performance. Recently, 2D-based heterojunction is getting popular for outstanding properties, such as special light collecting structure to enhance light harvest, intimate interface to facilitate charge transfer and separation, and large specific surface area to provide abundant reactive sites. Recently, some new 2D-based heterostructures materials (both structure and composition) have been developed with excellent performance. 2D materials exert structural and functional advantages in these fine composite photocatalysts. In this review, the literatures about the photocatalytic conversion of CO2 are mainly summarized based on overall structure, interface type and material type of 2D-based heterojunction, with special attention given to the preparation, characterization, structural advantages and reaction mechanism of novel 2D-based heterojunction. This work is in hope of offering a basis for designing improved composite photocatalyst for CO2 photoreduction. 

Two-dimensional heterostructures for photocatalytic CO2 reduction.

Black phosphorus (BP) is always regarded as a potential electrocatalyst for the oxygen evolution reaction (OER) due to its extremely high carrier mobility and tunable electronic structure. However, the instability and poor intrinsic activity under ambient conditions greatly limit the further improvement of its OER performance. Herein, by coupling BP with nickel cobaltite with the aid of dry ball-milling, nickel cobaltite/BP (NCO/BP) heterostructures were rationally designed for alkaline OER catalysis. The NCO/BP heterostructures with interfacial P–M and P–O–M (M = Ni or Co) bonds significantly promote interfacial electron transfer and balance the adsorption of oxygen-containing intermediates, thus enhancing the electrocatalytic OER performance. The NCO/BP heterostructure exhibits an ultra-low overpotential of 197 mV at a current density of 10 mA·cm–2 and good electrocatalytic stability in alkaline media. By combining in situ Raman and DFT calculation analyses, the Ni sites may be the main active sites, and the interfacial P–M and P–O–M (M = Ni or Co) bonds significantly play a positive role in improving the electrocatalytic OER activity. This work fully confirms that the construction of heterostructures for interfacial electron regulation is a very promising way to emerging BP-based electrocatalysts. 

Interfacial Electronic Modulation on Nickel Cobaltite/Black Phosphorus Heterostructures for Boosting the Electrocatalytic Oxygen Evolution Reaction

The practicality of electrochemical water-splitting technology relies on the development of novel and efficient bifunctional electrocatalysts capable of facilitating both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER). Black phosphorus (BP) holds tremendous promise for HER and OER electrocatalysis owing to its fully exposed atoms and high carrier mobility. However, the electrocatalytic performance of BP is still much lower than the expected theoretical limit, presenting an exciting challenge for further advancements. Herein, we embed electrochemically exfoliated few-layer BP nanosheets in higher Fermi level (EF) of cobalt, nitrogen co-doped carbons to form a new heterojunction (CoNC-BP), as efficient bifunctional electrocatalysts toward HER and OER for the advancement overall water splitting applications. A directed interfacial electron transfer is realized from CoNC to BP, facilitated by the lowering Fermi level (EF). This interfacial electron transfer plays a crucial role in optimizing the adsorption and desorption of active intermediates, while also introducing an abundance of hypervalent Co sites. These factors collectively contribute to the remarkable electrocatalytic activities of HER and OER performance, leading to the efficient performance of the developed CoNC-BP heterojunction in water-splitting applications. This work demonstrates a promising breakthrough that can inspire the design of high-efficiency catalysts. 

Charge transfer interfaces across black phosphorus/Co, N Co-doped carbon heterojunction for enhanced electrocatalytic water splitting

Synthesis of Ni2P/Ni5P4 on porous N decorated rGO foam for efficiently electrocatalytic hydrogen evolution reaction

Facile in-situ electrochemical fabrication of highly efficient nickel hydroxide-iron hydroxide/graphene hybrid for oxygen evolution reaction

To acquire low-cost efficient electrocatalyst for oxygen evolution reaction (OER), a cobalt-iron oxide/graphene hybrid (Co-Fe/G) is fabricated by a facile three-electrode synthesis method. In the course of electrosynthesis, the exfoliation...

Electrochemical fabrication of efficient cobalt-iron oxide/graphene heterostructure by a three-electrode system for electrocatalytic oxygen evolution reaction

Abstract Highly active, stable, and cut-price (photo-)electrocatalysts are desired to overwhelm high energy barriers for anodic oxygen evolution reaction processes. Herein, a heterostructure of cobalt-iron oxide/black phosphorus nanosheets is in-situ synthesized via a facile and novel three-electrode electrolysis method. Bulky black phosphorus is exfoliated into its nanosheets at the cathode while the CoFe oxide is derived directly from the metal wire anode during the electrolysis process. This heterostructure exhibits excellent electrocatalytic oxygen evolution reaction (OER) performance, and the overpotential at 10 mA·cm −2 is 51 mV lower than that of the commercial RuO 2 catalyst. Its superior OER performance stems from the favorable adsorption behavior and an enlarged electrochemical active surface area of the catalyst. To reveal the origin of excellent OER performance from the point of adsorption strength of OH*, methanol oxidation reaction (MOR) test is applied under the identified OER operating conditions. Further introduction of light illumination enhances the OER activity of this heterostructure. The overpotential drops down to 280 mV, benefiting from pronounced photochemical response of black phosphorus nanosheets and iron oxide inside the heterostructure. This work develops a new electrochemical method to construct high performance and light-sensitive heterostructures from black phosphorus nanosheets for the OER. 

/pdf/cobalt-iron-oxide-black-phosphorus-nanosheet-heterostructure-229871wf.pdf

Cobalt-iron oxide/black phosphorus nanosheet heterostructure: Electrosynthesis and performance of (photo-)electrocatalytic oxygen evolution

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Facile in-situ electrochemical fabrication of highly efficient nickel hydroxide-iron hydroxide/graphene hybrid for oxygen evolution reaction

Electrochemical fabrication of efficient cobalt-iron oxide/graphene heterostructure by a three-electrode system for electrocatalytic oxygen evolution reaction

Cobalt-iron oxide/black phosphorus nanosheet heterostructure: Electrosynthesis and performance of (photo-)electrocatalytic oxygen evolution