Reduced Graphene Oxide‐Wrapped Co9–xFexS8/Co,Fe‐N‐C Composite as Bifunctional Electrocatalyst for Oxygen Reduction and Evolution

Searching for highly efficient bifunctional electrocatalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) using nonnoble metal‐based catalysts is essential for the development of many energy conversion systems, including rechargeable fuel cells and metal–air batteries. Here, Co_9–xFe_xS₈/Co,Fe‐N‐C hybrids wrapped by reduced graphene oxide (rGO) (abbreviated as S‐Co_9–xFe_xS₈@rGO) are synthesized through a semivulcanization and calcination method using graphene oxide (GO) wrapped bimetallic zeolite imidazolate framework (ZIF) Co,Fe‐ZIF (CoFe‐ZIF@GO) as precursors. Benefiting from the synergistic effect of OER active CoFeS and ORR active Co,Fe‐N‐C in a single component, as well as high dispersity and enhanced conductivity derived from rGO coating and Fe‐doping, the obtained S‐Co_9–xFe_xS₈@rGO‐10 catalyst shows an ultrasmall overpotential of ≈0.29 V at 10 mA cm^?2 in OER and a half‐wave potential of 0.84 V in ORR, combining a superior oxygen electrode activity of ≈0.68 V in 0.1 m KOH.     

Enlarged CoO Covalency in Octahedral Sites Leading to Highly Efficient Spinel Oxides for Oxygen Evolution Reaction

Cobalt‐containing spinel oxides are promising electrocatalysts for the oxygen evolution reaction (OER) owing to their remarkable activity and durability. However, the activity still needs further improvement and related fundamentals remain untouched. The fact that spinel oxides tend to form cation deficiencies can differentiate their electrocatalysis from other oxide materials, for example, the most studied oxygen‐deficient perovskites. Here, a systematic study of spinel ZnFe_xCo_2?xO₄ oxides (x = 0–2.0) toward the OER is presented and a highly active catalyst superior to benchmark IrO₂ is developed. The distinctive OER activity is found to be dominated by the metal–oxygen covalency and an enlarged Co?O covalency by 10–30 at% Fe substitution is responsible for the activity enhancement. While the pH‐dependent OER activity of ZnFe_0.4Co_1.6O₄ (the optimal one) indicates decoupled proton–electron transfers during the OER, the involvement of lattice oxygen is not considered as a favorable route because of the downshifted O p‐band center relative to Fermi level governed by the spinel's cation deficient nature.     

Ultrathin Iron‐Cobalt Oxide Nanosheets with Abundant Oxygen Vacancies for the Oxygen Evolution Reaction

Electrochemical water splitting is a promising method for storing light/electrical energy in the form of H₂ fuel; however, it is limited by the sluggish anodic oxygen evolution reaction (OER). To improve the accessibility of H₂ production, it is necessary to develop an efficient OER catalyst with large surface area, abundant active sites, and good stability, through a low‐cost fabrication route. Herein, a facile solution reduction method using NaBH₄ as a reductant is developed to prepare iron‐cobalt oxide nanosheets (Fe_x Co_y ‐ONSs) with a large specific surface area (up to 261.1 m² g^?1), ultrathin thickness (1.2 nm), and, importantly, abundant oxygen vacancies. The mass activity of Fe₁Co₁‐ONS measured at an overpotential of 350 mV reaches up to 54.9 A g^?1, while its Tafel slope is 36.8 mV dec^?1; both of which are superior to those of commercial RuO₂, crystalline Fe₁Co₁‐ONP, and most reported OER catalysts. The excellent OER catalytic activity of Fe₁Co₁‐ONS can be attributed to its specific structure, e.g., ultrathin nanosheets that could facilitate mass diffusion/transport of OH^? ions and provide more active sites for OER catalysis, and oxygen vacancies that could improve electronic conductivity and facilitate adsorption of H₂O onto nearby Co³⁺ sites.     

Boosting Oxygen Evolution Reaction by Creating Both Metal Ion and Lattice-Oxygen Active Sites in a Complex Oxide

Developing efficient and low-cost electrocatalysts for the oxygen evolution reaction (OER) is of paramount importance to many chemical and energy transformation technologies. The diversity and flexibility of metal oxides offer numerous degrees of freedom for enhancing catalytic activity by tailoring their physicochemical properties, but the active site of current metal oxides for OER is still limited to either metal ions or lattice oxygen. Here, a new complex oxide with unique hexagonal structure consisting of one honeycomb-like network, Ba₄Sr₄(Co_0.8Fe_0.2)₄O₁₅ (hex-BSCF), is reported, demonstrating ultrahigh OER activity because both the tetrahedral Co ions and the octahedral oxygen ions on the surface are active, as confirmed by combined X-ray absorption spectroscopy analysis and theoretical calculations. The bulk hex-BSCF material synthesized by the facile and scalable sol–gel method achieves 10 mA cm⁻² at a low overpotential of only 340 mV (and small Tafel slope of 47 mV dec⁻¹) in 0.1 m KOH, surpassing most metal oxides ever reported for OER, while maintaining excellent durability. This study opens up a new avenue to dramatically enhancing catalytic activity of metal oxides for other applications through rational design of structures with multiple active sites.     

Co9S8 Nanoparticles‐Embedded N/S‐Codoped Carbon Nanofibers Derived from Metal–Organic Framework‐Wrapped CdS Nanowires for Efficient Oxygen Evolution Reaction

Metal–organic frameworks (MOFs) with tunable compositions and morphologies are recognized as efficient self‐sacrificial templates to achieve function‐oriented nanostructured materials. Moreover, it is urgently needed to develop highly efficient noble metal‐free oxygen evolution reaction (OER) electrocatalysts to accelerate the development of overall water splitting green energy conversion systems. Herein, a facile and cost‐efficient strategy to synthesize Co₉S₈ nanoparticles‐embedded N/S‐codoped carbon nanofibers (Co₉S₈/NSCNFs) as highly active OER catalyst is developed. The hybrid precursor of core–shell ZIF‐wrapped CdS nanowires is first prepared and then leads to the formation of uniformly dispersed Co₉S₈/N, S‐codoped carbon nanocomposites through a one‐step calcination reaction. The optimal Co₉S₈/NSCNFs‐850 is demonstrated to possess excellent electrocatalytic performance for OER in 1.0 m KOH solution, affording a low overpotential of 302 mV to reach the current density of 10 mA cm^?2, a small Tafel slope of 54 mV dec^?1, and superior long‐term stability for 1000 cyclic voltammetry cycles. The favorable results raise a concept of exploring more MOF‐based nanohybrids as precursors to induce the synthesis of novel porous nanomaterials as non‐noble‐metal electrocatalysts for sustainable energy conversion.     

Enlarged Co?O Covalency in Octahedral Sites Leading to Highly Efficient Spinel Oxides for Oxygen Evolution Reaction

Cobalt‐containing spinel oxides are promising electrocatalysts for the oxygen evolution reaction (OER) owing to their remarkable activity and durability. However, the activity still needs further improvement and related fundamentals remain untouched. The fact that spinel oxides tend to form cation deficiencies can differentiate their electrocatalysis from other oxide materials, for example, the most studied oxygen‐deficient perovskites. Here, a systematic study of spinel ZnFe_xCo_2?xO₄ oxides (x = 0–2.0) toward the OER is presented and a highly active catalyst superior to benchmark IrO₂ is developed. The distinctive OER activity is found to be dominated by the metal–oxygen covalency and an enlarged Co? O covalency by 10–30 at% Fe substitution is responsible for the activity enhancement. While the pH‐dependent OER activity of ZnFe_0.4Co_1.6O₄ (the optimal one) indicates decoupled proton–electron transfers during the OER, the involvement of lattice oxygen is not considered as a favorable route because of the downshifted O p‐band center relative to Fermi level governed by the spinel's cation deficient nature.     

Variable range hopping conduction of polaron in n = 2 Ruddlesden–Popper phase Sr3Fe1.5Co0.5O6.77

A Ruddlesden–Popper type Sr₃Fe_1.5Co_0.5O_7−δ ceramic was synthesized under air. The sample was found to have a slight oxygen deficiency, δ, of around 0.23. The crystal structure was determined to be a perovskite structure with tetragonal space group I4/mmm. The dependence of resistivity on temperature showed that electronic transport in Sr₃Fe_1.5Co_0.5O_6.77 is well described by a variable range hopping conduction mechanism.     

One‐Step Route Synthesized Co2P/Ru/N‐Doped Carbon Nanotube Hybrids as Bifunctional Electrocatalysts for High‐Performance Li–O2 Batteries

The large‐scale commercial application of lithium–oxygen batteries (LOBs) is overwhelmed by the sluggish kinetics of oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) associated with insoluble and insulated Li₂O₂. Herein, an elaborate design on a highly catalytic LOBs cathode constructed by N‐doped carbon nanotubes (CNT) with in situ encapsulated Co₂P and Ru nanoparticles is reported. The homogeneously dispersed Co₂P and Ru catalysts can effectively modulate the formation and decomposition behavior of Li₂O₂ during discharge/charge processes, ameliorating the electronically insulating property of Li₂O₂ and constructing a homogenous low‐impedance Li₂O₂/catalyst interface. Compared with Co/CNT and Ru/CNT electrodes, the Co₂P/Ru/CNT electrode delivers much higher oxygen reduction triggering onset potential and higher ORR and OER peak current and integral areas, showing greatly improved ORR/OER kinetics due to the synergistic effects of Co₂P and Ru. Li–O₂ cells based on the Ru/Co₂P/CNT electrode demonstrate improved ORR/OER overpotential of 0.75 V, excellent rate capability of 12 800 mAh g^?1 at 1 A g^?1, and superior cycle stability for more than 185 cycles under a restricted capacity of 1000 mAh g^?1 at 100 mA g^?1. This work paves an exciting avenue for the design and construction of bifunctional catalytic cathodes by coupling metal phosphides with other active components in LOBs.     

La0.6Sr0.4Co0.2Fe0.79M0.01O3−δ (M = Ni,Pd) perovskites synthesized by Citrate-EDTA method: Oxygen vacancies effect on electrochemical properties

La_0.6Sr_0.4Co_0.2Fe_0.8O_3?δ (LSCF08), La_0.6Sr_0.4Co_0.2Fe_0.79Ni_0.01O_3?δ (LSCF08-Ni) and La_0.6Sr_0.4Co_0.2Fe_0.79Pd_0.01O_3?δ (LSCF08-Pd) perovskites were synthesized by Citrate-EDTA method, by using NiCl₂ or PdCl₂ as metal precursors, and their physicochemical properties were characterized by XRD, TGA, TPD and TPR. XRD data evidenced an expansion of the lattice parameters of LSCF08-Pd, while a contraction of the lattice occurred for LSCF08-Ni, with respect to the undoped LSCF, suggesting different oxygen vacancies content in the perovskite (confirmed by TGA) likely due to a different oxidation state of Ni and Pd species stabilized in the structure.TEM analyses performed over LSCF08-Pd revealed the presence of metallic Pd nanoparticles well dispersed in the matrix that accounts for the increased reducibility of the Co and Fe species with respect to LSCF08-Ni and undoped perovskite. AC impedance measurements that were carried out on symmetric cells consisting of LSCF-based materials deposited onto Ce_0.8Gd_0.2O_2?δ (GDC) electrolyte proved the enhanced electrochemical performances of Ni/Pd doped LSCF.The electrochemical characterization of LSCF08, LSCF08-Ni and LSCF08-Pd electrodes was completed by performing cyclic voltammetry experiments in the range of temperature 600–800?°C, varying the potential (U) between 0.3?V and ?1?V, at scan rates in the range 1–50?mV?s^?1 and working under flow of 0.7?vol% O₂ in He (30?ml/min).     

Super‐Exchange Interaction Induced Overall Optimization in Ferromagnetic Perovskite Oxides Enables Ultrafast Water Oxidation

Oxygen evolution reaction (OER) is crucial in many renewable electrochemical technologies including regenerative fuel cells, rechargeable metal–air batteries, and water splitting. It is found that abundant active sites with favorable electronic structure and high electrical conductivity play a dominant role in achieving high electrocatalytic efficiency of perovskites, thus efficient strategies need to be designed to generate multiple beneficial factors for OER. Here, highlighted is an unusual super‐exchange effect in ferromagnetic perovskite oxide to optimize active sites and enhance electrical conductivity. A systematic exploration about the composition‐dependent OER activity in SrCo_1x Ru_x O_3?δ (denoted as SCRx) (x = 0.0–1.0) perovskite is displayed with special attention on the role of super‐exchange interaction between high spin (HS) Co³⁺ and Ru⁵⁺ ions. Induced by the unique Co³⁺–O–Ru⁵⁺ super‐exchange interactions, the SCR0.1 is endowed with abundant OER active species including Co³⁺/Co⁴⁺, Ru⁵⁺, and O₂^2?/O^?, high electrical conductivity, and metal–oxygen covalency. Benefiting from these advantageous factors for OER electrocatalysis, the optimized SCR0.1 catalyst exhibits a remarkable activity with a low overpotential of 360 mV at 10 mA cm^?2, which exceeds the benchmark RuO₂ and most well‐known perovskite oxides reported so far, while maintaining excellent durability. This work provides a new pathway in developing perovskite catalysts for efficient catalysis.     

Ultrafine Co3O4 Nanoparticles within Nitrogen‐Doped Carbon Matrix Derived from Metal–Organic Complex for Boosting Lithium Storage and Oxygen Evolution Reaction

Transition metal oxides have recently received great attention for application in advanced lithium‐ion batteries (LIBs) and oxygen evolution reaction (OER). Herein, the ethylenediaminetetraacetic cobalt complex as a precursor to synthesize ultrafine Co₃O₄ nanoparticles encapsulated into a nitrogen‐doped carbon matrix (NC) composites is presented. The as‐prepared Co₃O₄/NC‐350 obtained by pyrolysis at 350 °C demonstrates superior rate performance (372 mAh g^?1 at 5.0 A g^?1) and high cycling stability (92% capacity retention after 300 cycles at 1.0 A g^?1) as anode for LIBs. When evaluated as an electrocatalyst for OER, the Co₃O₄/NC‐350 achieves an overpotential of 298 mV at a current density of 10 mA cm^?2. The NC‐encapsualted porous hierarchical structure assures fast and continuous electron transportation, high activity sites, and strong structural integrity. This works offers novel complex precursors for synthesizing transition metal–based electrodes for boosting electrochemical energy conversion and storage.     

Amorphous Bimetallic Oxide–Graphene Hybrids as Bifunctional Oxygen Electrocatalysts for Rechargeable Zn–Air Batteries

Metal oxides of earth‐abundant elements are promising electrocatalysts to overcome the sluggish oxygen evolution and oxygen reduction reaction (OER/ORR) in many electrochemical energy‐conversion devices. However, it is difficult to control their catalytic activity precisely. Here, a general three‐stage synthesis strategy is described to produce a family of hybrid materials comprising amorphous bimetallic oxide nanoparticles anchored on N‐doped reduced graphene oxide with simultaneous control of nanoparticle elemental composition, size, and crystallinity. Amorphous Fe_0.5Co_0.5O_x is obtained from Prussian blue analog nanocrystals, showing excellent OER activity with a Tafel slope of 30.1 mV dec^?1 and an overpotential of 257 mV for 10 mA cm^?2 and superior ORR activity with a large limiting current density of ?5.25 mA cm^?2 at 0.6 V. A fabricated Zn–air battery delivers a specific capacity of 756 mA h g_Zn^?1 (corresponding to an energy density of 904 W h kg_Zn^?1), a peak power density of 86 mW cm^?2 and can be cycled over 120 h at 10 mA cm^?2. Other two amorphous bimetallic, Ni_0.4Fe_0.6O_x and Ni_0.33Co_0.67O_x , are also produced to demonstrate the general applicability of this method for synthesizing binary metal oxides with controllable structures as electrocatalysts for energy conversion.     

2D Electron Gas and Oxygen Vacancy Induced High Oxygen Evolution Performances for Advanced Co3O4/CeO2 Nanohybrids

The rational design of atomic‐scale interfaces in multiphase nanohybrids is an alluring and challenging approach to develop advanced electrocatalysts. Herein, through the selection of two different metal oxides with particular intrinsic features, advanced Co₃O₄/CeO₂ nanohybrids (NHs) with CeO₂ nanocubes anchored on Co₃O₄ nanosheets are developed, which show not only high oxygen vacancy concentration but also remarkable 2D electron gas (2DEG) behavior with ≈0.79 ± 0.1 excess e^?/u.c. on the Ce³⁺ sites at the Co₃O₄–CeO₂ interface. Such a 2DEG transport channel leads to a high carrier density of 3.8 × 10¹⁴ cm^?2 and good conductivity. Consequently, the Co₃O₄/CeO₂ NHs demonstrate dramatically enhanced oxygen evolution reaction (OER) performances with a low overpotential of 270 mV at 10 mA cm^?2 and a high turnover frequency of 0.25 s^?1 when compared to those of pure Co₃O₄ and CeO₂ counterparts, outperforming commercial IrO₂ and some recently reported representative OER catalysts. These results demonstrate the validity of tailoring the electrocatalytic properties of metal oxides by 2DEG engineering, offering a step forward in the design of advanced hybrid nanostructures.     

Defects‐Induced In‐Plane Heterophase in Cobalt Oxide Nanosheets for Oxygen Evolution Reaction

Cobalt oxides as efficient oxygen evolution reaction (OER) electrocatalysts have received much attention because of their rich reserves and cheap cost. There are two common cobalt oxides, Co₃O₄ (spinel phase, stable but poor intrinsic activity) and CoO (rocksalt phase, active but easily be oxidatized). Constructing Co₃O₄/CoO heterophase can inherit both characteristic features of each component and form a heterophase interface facilitating charge transfer, which is believed to be an effective strategy in designing excellent electrocatalysts. Herein, an atomic arrangement engineering strategy is applied to improve electrocatalytic activity of Co₃O₄ for the OER. With the presence of oxygen vacancies, cobalt atoms at tetrahedral sites in Co₃O₄ can more easily diffuse into interstitial octahedral sites to form CoO phase structure as revealed by periodic density functional theory computations. The Co₃O₄/CoO spinel/rocksalt heterophase can be in situ fabricated at the atomic scale in plane. The overpotential to reach 10 mA cm^?2 of Co₃O₄/CoO is 1.532 V, which is 92 mV smaller than that of Co₃O₄. Theoretical calculations confirm that the excellent electrochemical activity is corresponding to a decline in average p‐state energy of adsorbed‐O on the Co₃O₄/CoO heterophase interface. The reaction Gibbs energy barrier has been significantly decreased with the construction of the heterophase interface.     

Defect Engineering of Chalcogen‐Tailored Oxygen Electrocatalysts for Rechargeable Quasi‐Solid‐State Zinc–Air Batteries

A critical bottleneck limiting the performance of rechargeable zinc–air batteries lies in the inefficient bifunctional electrocatalysts for the oxygen reduction and evolution reactions at the air electrodes. Hybridizing transition‐metal oxides with functional graphene materials has shown great advantages due to their catalytic synergism. However, both the mediocre catalytic activity of metal oxides and the restricted 2D mass/charge transfer of graphene render these hybrid catalysts inefficient. Here, an effective strategy combining anion substitution, defect engineering, and the dopant effect to address the above two critical issues is shown. This strategy is demonstrated on a hybrid catalyst consisting of sulfur‐deficient cobalt oxysulfide single crystals and nitrogen‐doped graphene nanomeshes (CoO_0.87S_0.13/GN). The defect chemistries of both oxygen‐vacancy‐rich, nonstoichiometric cobalt oxysulfides and edge‐nitrogen‐rich graphene nanomeshes lead to a remarkable improvement in electrocatalytic performance, where CoO_0.87S_0.13/GN exhibits strongly comparable catalytic activity to and much better stability than the best‐known benchmark noble‐metal catalysts. In application to quasi‐solid‐state zinc–air batteries, CoO_0.87S_0.13/GN as a freestanding catalyst assembly benefits from both structural integrity and enhanced charge transfer to achieve efficient and very stable cycling operation over 300 cycles with a low discharge–charge voltage gap of 0.77 V at 20 mA cm^?2 under ambient conditions.     

An Amorphous Nickel–Iron‐Based Electrocatalyst with Unusual Local Structures for Ultrafast Oxygen Evolution Reaction

Rationally designing active and durable catalysts for the oxygen evolution reaction (OER) is of primary importance in water splitting. Perovskite oxides (ABO₃) with versatile structures and multiple physicochemical properties have triggered considerable interest in the OER. The leaching of A site cations can create nanostructures and amorphous motifs on the perovskite matrix, thus facilitating the OER process. However, selectively dissolving A site cations and simultaneously obtaining more active amorphous motifs derived from the B site cations remains a great challenge. Herein, a top‐down strategy is proposed to transform bulk crystalline perovskite (LaNiO₃) into a nanostructured amorphous hydroxide by FeCl₃ post‐treatment, resulting in an extremely low overpotential of 189 mV at 10 mA cm^?2. The top‐down‐constructed amorphous catalyst with a large surface area has dual NiFe active sites, where high‐valence Ni³⁺‐based edge‐sharing octahedral frameworks are surrounded by interstitial distorted Fe octahedra and contribute to the superior OER performance. This top‐down strategy provides a valid way to design novel perovskite‐derived catalysts.     

Ni‐Fe Nitride Nanoplates on Nitrogen‐Doped Graphene as a Synergistic Catalyst for Reversible Oxygen Evolution Reaction and Rechargeable Zn‐Air Battery

Obtaining bifunctional electrocatalysts with high activity for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is a main hurdle in the application of rechargeable metal‐air batteries. Earth‐abundant 3d transition metal‐based catalysts have been developed for the OER and ORR; however, most of these are based on oxides, whose insulating nature strongly restricts their catalytic performance. This study describes a metallic Ni‐Fe nitride/nitrogen‐doped graphene hybrid in which 2D Ni‐Fe nitride nanoplates are strongly coupled with the graphene support. Electronic structure of the Ni‐Fe nitride is changed by hybridizing with the nitrogen‐doped graphene. The unique heterostructure of this hybrid catalyst results in very high OER activity with the lowest onset overpotential (150 mV) reported, and good ORR activity comparable to that for commercial Pt/C. The high activity and durability of this bifunctional catalyst are also confirmed in rechargeable zinc‐air batteries that are stable for 180 cycles with an overall overpotential of only 0.77 V at 10 mA^?2.     

Pseudocapacitive Ni‐Co‐Fe Hydroxides/N‐Doped Carbon Nanoplates‐Based Electrocatalyst for Efficient Oxygen Evolution

The oxygen evolution reaction (OER) catalytic activity of a transition metal oxides/hydroxides based electrocatalyst is related to its pseudocapacitance at potentials lower than the OER standard potential. Thus, a well‐defined pseudocapacitance could be a great supplement to boost OER. Herein, a highly pseudocapacitive Ni‐Fe‐Co hydroxides/N‐doped carbon nanoplates (NiCoFe‐NC)‐based electrocatalyst is synthesized using a facile one‐pot solvothermal approach. The NiCoFe‐NC has a great pseudocapacitive performance with 1849 F g^?1 specific capacitance and 31.5 Wh kg^?1 energy density. This material also exhibits an excellent OER catalytic activity comparable to the benchmark RuO₂ catalysts (an initiating overpotential of 160 mV and delivering 10 mA cm^?2 current density at 250 mV, with a Tafel slope of 31 mV dec^?1). The catalytic performance of the optimized NiCoFe‐NC catalyst could keep 24 h. X‐ray photoelectron spectroscopy, electrochemically active surface area, and other physicochemical and electrochemical analyses reveal that its great OER catalytic activity is ascribed to the Ni‐Co hydroxides with modular 2‐Dimensional layered structure, the synergistic interactions among the Fe(III) species and Ni, Co metal centers, and the improved hydrophily endowed by the incorporation of N‐doped carbon hydrogel. This work might provide a useful and general strategy to design and synthesize high‐performance metal (hydr)oxides OER electrocatalysts.     

Ultrathin Ruddlesden–Popper Perovskite Heterojunction for Sensitive Photodetection

Thanks to their unique optical and electric properties, 2D materials have attracted a lot of interest for optoelectronic applications. Here, the emerging 2D materials, organic–inorganic hybrid perovskites with van der Waals interlayer interaction (Ruddlesden–Popper perovskites), are synthesized and characterized. Photodetectors based on the few‐layer Ruddlesden–Popper perovskite show good photoresponsivity as well as good detectivity. In order to further improve the photoresponse performance, 2D MoS₂ is chosen to construct the perovskite–MoS₂ heterojunction. The performance of the hybrid photodetector is largely improved with 6 and 2 orders of magnitude enhancement for photoresponsivity (10⁴ A W^?1) and detectivity (4 × 10¹⁰ Jones), respectively, which demonstrates the facile charge separation at the interface between perovskite and MoS₂. Furthermore, the contribution of back gate tuning is proved with a greatly reduced dark current. The results demonstrated here will open up a new field for the investigation of 2D perovskites for optoelectronic applications.