Green Energy Conversion Research Articles

Na-doped cobalt spinel electrocatalysts prepared by programmed electrostatic spraying for improving OER activity and durability in acidic media

The daunting challenge to establish a trade-off among the activity, durability, and cost of electrocatalysts for oxygen evolution reaction (OER) with sluggish reaction kinetics impedes the practical green energy conversion. Hereby, a non-noble metal-based electrocatalyst (i.e., Na-doped Co3O4) was in-situ prepared by programmed electrostatic spraying as an advanced alternative to the costly and scarce state-of-the-art IrO2 and RuO2-based electrocatalysts. The utilization of this sprayer facilitates intimate contact with the substrate electrode and provides short ion diffusion paths, facilitating efficient electron transport. Additionally, the doping of Na ions into the Co3O4 structure results in structural distortion and charge redistribution, leading to the generation of oxygen vacancies (OVs). These OVs enhance the activity of lattice oxygen atoms, thus enabling rapid and durable oxygen evolution in an acidic media (0.5 M H2SO4). The optimal Na-Co3O4 (AA) exhibits a notably low overpotential of 360 mV@10 mA·cm−2 and at least 200 h stability. In addition, density functional theory (DFT) calculations confirm that the incorporation of Na ions significantly elevates electrical conductivity by decreasing the energy band gap and reduces the free energy barrier for the conversion of *O to *OOH, thereby improving the intrinsic OER activity. Finally, by implanting the catalyst in a single-cell proton exchange membrane water electrolyzer (PEMWE), the current density of 100 mA·cm−2 is achieved at a voltage of 1.62 V. This innovative non-noble metal catalyst holds great potential for scalable PEMWE anodes.

Rational construction of N-containing carbon sheets atomically doped NiP-CoP nanohybrid electrocatalysts for enhanced green hydrogen and oxygen production

The pursuit of sustainable energy production has directed rigorous research in the field of electrocatalysis, particularly for water electrolysis (i.e., hydrogen (HER) and oxygen evolution reactions (OER)). This study discloses the rational synthesis of N-containing carbon sheets atomically doped NiP-CoP nanohybrid (NiP-CoP/NCS) via precipitation/calcination. The fabrication method tailored the physicochemical merits for collective contribution to improved green hydrogen and oxygen, elucidated by surface/bulk characterization and theoretical calculations. Thus, the NiP-CoP/NCS had improved HER activity at lower overpotential (ƞ10 = 197.7/274.6 mV), higher exchange current density (jo = 0.71/0.67 mA/cm2), turnover frequency (TOF = 2.63/1.47 s-1), H2 production rate (3601.63/2519.12 µmol/g/h) and superior stability after 24 h in acid/alkaline media, than NiP/NCS and CoP/NCS. Moreover, NiP-CoP/NCS delivered impressive OER activity at reduced ƞ10 (309.1 mV), and Tafel slope (ba = 58.9 ± 3.0 mV/dec), but higher TOF (3.67 s-1) and O2 production rate (3643.96 µmol/g/h) relative to NiP/NCS and CoP/NCS, besides higher stability for 24 h. These were further proved by theoretical calculations. This work indicates a deeper understanding of the fabrication methods of making efficient electrocatalysts for green and sustainable energy conversion.

First principles study of V2CT2-based MXenes materials in oxygen reduction and oxygen evolution reactions

The development of bifunctional ORR/OER electrocatalysts with low cost, high activity and sustainable cycle plays an important role in improving the performance of new green energy storage and conversion devices to alleviate the energy crisis and environmental pollution. As a graphene-like two-dimensional inorganic layered compound with unique electrochemistry, MXenes materials have attracted more and more attention in the field of electrocatalytic applications. In this paper, based on the first-principles calculation method based on density functional theory (DFT) and quantum mechanics, an effective scheme for designing efficient ORR/OER bifunctional electrocatalysts by introducing Pd/Pt single atoms to regulate the electronic structure of V2CT2 (T = O, F) is proposed. Firstly, we discussed the stability of the designed series of single-atom catalysts by calculating the formation energy, binding energy and molecular dynamics simulation. Secondly, by comparing the theoretical overpotentials of these single-atom catalysts for ORR and OER, we found that among the designed SACs, V2CO2-Pd, V2CF2-Pd and V2CO2-VO-Pt are catalysts with good bifunctional catalytic activity for ORR/OER. Our work provides some guidance for the application of MXenes materials in the field of electrocatalysis.

Advancing flexible thermoelectrics for integrated electronics.

With the increasing demand for energy and the climate challenges caused by the consumption of traditional fuels, there is an urgent need to accelerate the adoption of green and sustainable energy conversion and storage technologies. The integration of flexible thermoelectrics with other various energy conversion technologies plays a crucial role, enabling the conversion of multiple forms of energy such as temperature differentials, solar energy, mechanical force, and humidity into electricity. The development of these technologies lays the foundation for sustainable power solutions and promotes research progress in energy conversion. Given the complexity and rapid development of this field, this review provides a detailed overview of the progress of multifunctional integrated energy conversion and storage technologies based on thermoelectric conversion. The focus is on improving material performance, optimizing the design of integrated device structures, and achieving device flexibility to expand their application scenarios, particularly the integration and multi-functionalization of wearable energy conversion technologies. Additionally, we discuss the current development bottlenecks and future directions to facilitate the continuous advancement of this field.

Cutting-edge technologies and recent modernization on multifunctional perovskite materials for green energy conversion and spintronic applications

This featured letter summarizes the recent developments in green energy and spintronic technologies based on multifunctional i.e., multiferroic (MF) and magnetoelectric (ME) materials. These are non-toxic materials, find applications in spintronic, non-volatile memory devices, microelectromechanical systems (MEMS), photovoltaics and next generation IC miniaturization devices. Recent studies on MF and ME materials have probed and analyzed significant properties such as evidence of photo-response and significant power conversion efficiency (PCE) of multiferroic-based solar cells (SCs), evidence of electro-caloric effect (ECE) which find usage in non-toxic solid state refrigeration devices, photo- and electro-catalytic activities for green hydrogen generation, magnon-phonon coupling and existence of magnon polarons which can facilitate spintronic device technology and thermal Hall effect and, hybrid nano-generators utilized to empower portable electronic devices. All such applications are comprehensively analyzed in-depth in this letter.

Computational Engineering of Non-van der Waals 2D Magnetene for Enhanced Oxygen Evolution and Reduction Reactions.

Non-van der Waals two-dimensional materials containing exposed transition metal atoms are promising catalysts for green energy storage and conversion. For instance, hematene and ilmenene have been successfully applied as catalysts. Building on these reports, this work is the first investigation of recently synthesized magnetene towards the Oxygen Evolution Reaction (OER) and Oxygen Reduction Reaction (ORR). Using Density Functional Theory (DFT) calculations, we unveil the mechanism, performance and ideal conditions for OER and ORR on magnetene. With overpotentials of ηOER = 0.50 V and ηORR = 0.41 V, the material is not only a bifunctional catalyst, but also superior to state-of-the-art systems such as Pt and IrO2. Additionally, its catalytic properties can be further enhanced through engineering strategies such as point defects and in-plane compression. It reaches ηORR = 0.28 V at a compressive strain of only 2%, while the presence of Ni boosts it to ηOER = 0.39 V and ηORR = 0.31 V, comparable to many reported single-atom catalysts. Overall, this work demonstrates that magnetene is a promising bifunctional catalyst for applications such as regenerative fuel cells and metal-air batteries.

Research on the Configuration of a 100% Green Electricity Supplied Zero-Carbon Integrated Energy Station

In the context of rapid growth in renewable energy installations and increasingly severe consumption issues, this paper designs a 100% green electricity supplied zero-carbon integrated energy station. It aims to analyze its configuration focusing on the following three core features: zero carbon emissions, 100% green electricity supply, and a centralized–distributed system structure. It discusses equipment selection and provides models for configuring upstream green electricity resources, power generation, energy storage, transformer, and energy conversion. The study examines the synergy between lithium-ion battery storage and modular molten salt thermal storage, along with the virtual energy storage characteristics formed by thermal load inertia, supported by mathematical models. Based on the data from a green electricity system in an Eastern Chinese city and typical load profiles, the paper validates a specific configuration for a 100% green electricity supplied zero-carbon integrated energy station, confirming model accuracy and calculating the required scale of upstream green electricity resources. It proves that establishing an electro-thermal storage synergy system is crucial for addressing the significant fluctuations in renewable energy output. It also argues that leveraging thermal load inertia to create virtual storage can reduce the investment in energy storage system construction.

Impact on green energy conversion and stability of PSC device with the insertion of bifunctional molecule as an interfacial layer

Organometallic-halide perovskite solar cells (PSCs) are currently considered the most promising solar cell devices for the next generation. PSCs utilizing formamidinium lead triiodide (FAPbI3) have showcased exceptional capabilities as an efficient light absorbers in the realm of thin-film photovoltaics. This study encompasses a comprehensive analysis of two device configurations: FTO/TiO2/FAPbI3/CBz-PAI/Spiro-OMeTAD/Au and FTO/TiO2/FAPbI3/Spiro-OMeTAD/Au through computational modeling and performance optimization. By introducing CBz-PAI as a defects passivation layer at the perovskite/Spiro-OMeTAD interface, we aim to enhance the performance and improve the stability of the above mentioned solar cell devices and examine the influence of the CBz-PAI layer. The performance of both devices was thoroughly analysed by examining the effect of variations in perovskite, electron transport layer (ETL), and hole transport layer (HTL) thickness, perovskite doping concentration and defect density, electron affinity as well as series and shunt resistance. Additionally, the impact of band gap and temperature on the devices were evaluated. Furthermore, different ETLs and HTLs were tested to optimize both device configurations and enhance their performance and stability. The simulation results revealed that the device architecture consisting of FTO/WS2/FAPbI3/CBz-PAI/CuI/Au exhibited the highest power conversion efficiency (PCE) among all the different configurations. The estimated values of open circuit voltage (VOC), short circuit current density (JSC), fill factor (FF) and PCE of the designed PSC were found to be 1.186 V, 28.19 mA/cm2, 80.57 % and 26.93 % respectively. Overall, this thorough simulation, supported by the validation results, demonstrated the capability of FAPbI3 absorber with CBz-PAI as defect passivator. WS2 and CuI as ETL and HTL, respectively, facilitating the pathway for the advancement of cost-effective, stable and efficient FAPbI3 PSCs in the photovoltaic industry.

Directional Growth and Density Modulation of Single‐Atom Platinum for Efficient Electrocatalytic Hydrogen Evolution

AbstractDispersion of single atoms (SAs) in the host is important for optimizing catalytic activity. Herein, we propose a novel strategy to tune oxygen vacancies in CeO2−X directionally anchoring the single atom platinum (PtSA), which is uniformly dispersed on the rGO. The catalyst's performance for the hydrogen evolution reaction (HER) can be enhanced by controlling different densities of CeO2‐X in rGO. The PtSA performs best optimally densified and loaded on homogeneous and moderately densified CeO2‐X/rGO (PtSA−M−CeO2−X/rGO). It exhibited higher activity in HER with an overpotential of 25 mV at 0.5 M H2SO4 and 33 mV at 1 KOH than that of almost reported electrocatalysts. Furthermore, it exhibited stability for 90 hours at −100 mA cm−2 in 1 KOH and −150 mA cm−2 in 0.5 M H2SO4 conditions, respectively. Through comprehensive experiments and theoretical calculations, the suitable dispersion density of PtSA on the defects of CeO2−X with more active sites gives the potential for practical applications. This research paves the way for developing single‐atom catalysts with exceptional catalytic activity and stability, holding promise in advanced green energy conversion through defects engineering.

Directional Growth and Density Modulation of Single-Atom Platinum for Efficient Electrocatalytic Hydrogen Evolution.

Dispersion of single atoms (SAs) in the host is important for optimizing catalytic activity. Herein, we propose a novel strategy to tune oxygen vacancies in CeO2-X directionally anchoring the single atom platinum (PtSA), which is uniformly dispersed on the rGO. The catalyst's performance for the hydrogen evolution reaction (HER) can be enhanced by controlling different densities of CeO2-X in rGO. The PtSA performs best optimally densified and loaded on homogeneous and moderately densified CeO2-X/rGO (PtSA-M-CeO2-X/rGO). It exhibited higher activity in HER with an overpotential of 25 mV at 0.5 M H2SO4 and 33 mV at 1 KOH than that of almost reported electrocatalysts. Furthermore, it exhibited stability for 90 hours at -100 mA cm-2 in 1 KOH and -150 mA cm-2 in 0.5 M H2SO4 conditions, respectively. Through comprehensive experiments and theoretical calculations, the suitable dispersion density of PtSA on the defects of CeO2-X with more active sites gives the potential for practical applications. This research paves the way for developing single-atom catalysts with exceptional catalytic activity and stability, holding promise in advanced green energy conversion through defects engineering.

Advances in green energy conversion efficiency and interfacial engineering investigations of lead-free FASnI3-based PSC device

Formamidinium tin iodide (HC(NH2)2SnI3– FASnI3) based lead-free perovskite solar cells (PSCs) have gained significant interest due to higher carrier mobility, wider band gap and superior device stability. However, limited device efficiency of FASnI3 based PSCs hindered its future adoption. Therefore, in the present study FASnI3 based PSC has been rigorously studied with TiO2 as electron transport layer (ETL) and Spiro-OMeTAD as hole transport layer (HTL). The PSC with cell configuration of FTO/TiO2/FASnI3/Spiro-OMeTAD/Au is designed computationally through the SCAPS simulation software to accomplish highest device efficiency. Detailed investigation and optimization have been performed in terms of thickness and bandgap of perovskite absorber, as well as temperature and series resistance of PSC device which further exhibited superior device efficiency with open circuit voltage (VOC) of 0.93V, current density (JSC) of 31.21 mA/cm2, fill factor (FF) of 83.37 % and the champion power conversion efficiency (PCE) of 24.20 %. In addition, the interfacial engineering investigations have been performed via. the capacitance-voltage (C–V), conductance-voltage (G-V) and Mott-Shottkey plots. These investigations have been performed through simulation approach and substantiate the efficiency of PSCs directly related to capacitance and scarcity of localized deep states within the FASnI3 absorber. Further, capacitance frequency (C-f) measurement under dark and illumination conditions confirmed the temperature-dependent response of the deep acceptor states and the influence of interface states on the overall performance of the device. Afterwards, Nyquist plots illustrate the predominant electrochemical impedance behavior, emphasizing the significant influence of the space charge region on the overall electrical response of the device and consistent semicircular patterns observed in all plots unequivocally confirms the dominance of the space charge region within the PSC heterostructure device. Such type of novel computational approach will be very useful to the experimentalists for the better efficiency device formation and helpful to the society to achieve the green energy requirements.

Sonication-Induced Boladipeptide-Based Metallogel as an Efficient Electrocatalyst for the Oxygen Evolution Reaction.

Bioinspired, self-assembled hybrid materials show great potential in the field of energy conversion. Here, we have prepared a sonication-induced boladipeptide (HO-YF-AA-FY-OH (PBFY); AA = Adipic acid, F = l-phenylalanine, and Y = l-tyrosine) and an anchored, self-assembled nickel-based coordinated polymeric nanohybrid hydrogel (Ni-PBFY). The morphological studies of hydrogels PBFY and Ni-PBFY exhibit nanofibrillar network structures. XPS analysis has been used to study the self-assembled coordinated polymeric hydrogel Ni-PBFY-3, with the aim of identifying its chemical makeup and electronic state. XANES and EXAFS analyses have been used to examine the local electronic structure and coordination environment of Ni-PBFY-3. The xerogel of Ni-PBFY was used to fabricate the electrodes and is utilized in the OER (oxygen evolution reaction). The native hydrogel (PBFY) contains a gelator boladipeptide of 15.33 mg (20 mmol L-1) in a final volume of 1 mL. The metallo-hydrogel (Ni-PBFY-3) is prepared by combining 15.33 mg (20 mmol L-1) of boladipeptide (PBFY) with 3 mg (13 mmol L-1) of NiCl2·6H2O metal in a final volume of 1 mL. It displays an ultralow Tafel slope of 74 mV dec-1 and a lower overpotential of 164 mV at a 10 mA cm-2 current density in a 1 M KOH electrolyte, compared to other electrocatalysts under the same experimental conditions. Furthermore, the Ni-PBFY-3 electrocatalyst has been witnessed to be highly stable during 100 h of chronopotentiometry performance. To explore the OER mechanism in an alkaline medium, a theoretical calculation was carried out by employing the first-principles-based density functional theory (DFT) method. The computed results obtained by the DFT method further confirm that the Ni-PBFY-3 electrocatalyst has a high intrinsic activity toward the OER, and the value of overpotential obtained from the present experiment agrees well with the computed value of the overpotential. The biomolecule-assisted electrocatalytic results provide a new approach for designing efficient electrocatalysts, which could have significant implications in the field of green energy conversion.

GeC/SnSe2 van der waals heterostructure: A promising direct Z-scheme photocatalyst for overall water splitting with strong optical absorption, high solar-to-hydrogen energy conversion efficiency and superior catalytic activity

To alleviate the energy crisis and achieve green energy conversion, the heterojunctions that can be applied to the photocatalytic decomposition of water have attracted attention. In this paper, we design a novel two-dimensional GeC/SnSe2 heterostructure and investigate in detail the structural stability, electronic characteristics, photocatalytic activity and optical behavior as well as the effects due to the applied strain based on the first-principles. Firstly, the most stable γ-stacking mode is determined by combining energy comparison, thermodynamic and dynamic studies. Second, the analysis of electronic properties demonstrates that the GeC/SnSe2 heterostructure exhibits a type-II energy band arrangement and a direct Z-scheme photocatalytic mechanism. This pivotal aspect enhances the separation of photogenerated carriers at the interface and facilitates the active participation of the most proficient materials in oxidation-reduction processes during photocatalytic hydrolysis reactions. The hydrolysis reaction's Gibbs free energy shift demonstrates the GeC/SnSe2 heterostructure's superior photocatalytic activity in neutral and alkaline environments and can spontaneously carry out the overall hydrolysis reaction, and this outstanding ability is not affected by the −4% to 4% strain range. In addition, the GeC/SnSe2 heterostructure has outstanding solar-to-hydrogen efficiency (58.18%) and excellent light absorption capability (up to 4×105cm−1) within visible light. The implications of these discoveries point towards the direct Z-scheme GeC/SnSe2 heterostructure holds promise as an excellent candidate for photocatalytic water splitting applications.

Carbon-Based Composites for Oxygen Evolution Reaction Electrocatalysts: Design, Fabrication, and Application.

The four-electron oxidation process of the oxygen evolution reaction (OER) highly influences the performance of many green energy storage and conversion devices due to its sluggish kinetics. The fabrication of cost-effective OER electrocatalysts via a facile and green method is, hence, highly desirable. This review summarizes and discusses the recent progress in creating carbon-based materials for alkaline OER. The contents mainly focus on the design, fabrication, and application of carbon-based materials for alkaline OER, including metal-free carbon materials, carbon-based supported composites, and carbon-based material core-shell hybrids. The work presents references and suggestions for the rational design of highly efficient carbon-based OER materials.

Polyoxometalate coupled polymers induced molybdenum phosphide with large surface area for efficient hydrogen evolution

Developing highly active hydrogen evolution reaction (HER) electrocatalysts possesses great significance for the green renewable energy conversion and storage. Here, through the electrostatic attraction between polyoxometalate (PMo12) and ammonium polyphosphate (APP) and the coordination with polyallylamine hydrochloride (PAH), the precursor was constructed, and then nitrogen-doped graphite carbon layer-coated MoP active particles (MoP@NC) were successfully prepared by high temperature carbonization. For HER, the overpotential of η10 for MoP@NC is 119 and 126 mV in acidic and alkaline electrolyte. Furthermore, in alkaline solution, when the current density reaches a certain degree (≥110 mA cm−2), the hydrogen production activity of the catalysts are the same as that of the industrial Pt/C catalysts, or even have a slight advantage. The synergistic interaction of active particles (MoP) and graphitic carbon layers and high specific surface area ensure the excellent activity of HER. N-doped porous carbon layers also protect MoP@NC working for 24 h. Moreover, the catalysts prepared in the same experimental environment with ammonium molybdate as metal source also showed good HER performance in acidic and alkaline environments. This study opens a general way to develop earth-rich Mo-based phosphide electrocatalysts with high activity for hydrolysis applications.

Iron Active Center Coordination Reconstruction in Iron Carbide Modified on Porous Carbon for Superior Overall Water Splitting.

In this work, a novel liquid nitrogen quenching strategy is engineered to fulfill iron active center coordination reconstruction within iron carbide (Fe3C) modified on biomass-derived nitrogen-doped porous carbon (NC) for initiating rapid hydrogen and oxygen evolution, where the chrysanthemum tea (elm seeds, corn leaves, and shaddock peel, etc.) is treated as biomass carbon source within Fe3C and NC. Moreover, the original thermodynamic stability is changed through the corresponding force generated by liquid nitrogen quenching and the phase transformation is induced with rich carbon vacancies with the increasing instantaneous temperature drop amplitude. Noteworthy, the optimizing intermediate absorption/desorption is achieved by new phases, Fe coordination, and carbon vacancies. The Fe3C/NC-550 (550 refers to quenching temperature) demonstrates outstanding overpotential for hydrogen evolution reaction (26.3mV at -10 mAcm-2) and oxygen evolution reaction (281.4 mV at 10mAcm-2), favorable overall water splitting activity (1.57 V at 10 mAcm-2). Density functional theory (DFT) calculations further confirm that liquid nitrogen quenching treatment can enhance the intrinsic electrocatalytic activity efficiently by optimizing the adsorption free energy of reaction intermediates. Overall, the above results authenticate that liquid nitrogen quenching strategy open up new possibilities for obtaining highly active electrocatalysts for the new generation of green energy conversion systems.

Donor-acceptor covalent organic framework/ZnIn2S4 core-shell structure S-scheme heterostructure for efficient photocatalytic hydrogen evolution

Covalent organic frameworks (COFs) show promising prospect as the photocatalysts with advantages of exceptional light adsorption capability, large specific surface area, and adjustable band structure. However, COFs usually suffer from severe recombination of photogenerated carriers. Therefore, there is an urgent demand to design effective COF-based heterostructures to enhance the separation of carriers. In this work, a porphyrin-based COF with electron donor-acceptor structure is synthesized via condensation polymerization by using 5,10,15,20-tetrakis(4-aminophenyl)porphyrin (TAPPP) and N,N,N',N'-tetra(4-formylphenyl)benzidin (NFPBD) as the donor and acceptor, respectively. Subsequently, ZnIn2S4 (ZIS) are successfully in-situ grown on the surface of porphyrin-based COF, forming a novel core-shell structure. The in-situ synthesized ZIS with positive charges can be easily adsorbed on the negatively charged sites of the COF’s surface via the electrostatic interaction. This organic/inorganic hybrid COF-ZIS heterostructure exhibits a superior photocatalytic hydrogen evolution (PHE) rate of 695 μmol g−1 h−1, approximately three times higher than that of ZIS. The construction of COF-ZIS heterostructure plays an important role in enhancing the separation and transport of photogenerated carriers, which provides more electrons at the surface of ZIS to take part in proton reduction. Electron paramagnetic resonance spectra confirm the charge carriers transfer mode in the COF-ZIS heterostructure via an S-scheme mechanism. Moreover, upon loading Pt as the cocatalyst, the heterostructure achieves an effective PHE rate of 2711 μmol g−1 h−1 along with an exceptional stability. Additionally, the COF-ZIS heterostructure reaches up to 2.45% of apparent quantum efficiency at 400 nm. Notably, the average lifetime of the COF-ZIS heterostructure increases by 43.2% and 98.9% compared to that of ZIS and the COF individually, as observed through single-particle fluorescence spectroscopy. This work gives valuable inspiration into the building of donor-acceptor COF-based S-scheme heterostructures to achieve highly effective green energy conversion by aligning band structures.

Experimental study of diphenylmethane gasification with supercritical CO2

Supercritical carbon dioxide (SCCO2) gasification reaction is one of the current popular research fields with wide application prospects in green chemical synthesis, environmental protection and energy conversion. This work aimed to investigate the effects of different conditions on the gas–liquid-solid three-phase products during the reaction of SCCO2 gasification of diphenylmethane. As a result, the carbon gasification efficiency (CE) and the hydrogen gasification efficiency (HE) were 25.99 % and 21.97 % respectively at 700 ℃ for 40 min, in which the CO reached the maximum of 15.64 ± 0.16 mol/kg. As the temperature and residence time increased, the apparent morphology of solid products became more homogeneous. In addition, based on the theories of cleavage of free radicals, secondary cleavage of free radicals and binding of free radicals, three pathways for the generation of fluorene, biphenyl and m-terphenyl were postulated. The experimental results provide fundamental data and theoretical support for an in-depth understanding of the reactions mechanism under the SCCO2 atmosphere, which is of great significance for deepening our knowledge of supercritical carbon dioxide reduction reactions and promoting green chemical synthesis research.

Enhanced Electrocatalytic Oxygen Evolution by In Situ Growth of Tetrametallic Metal-Organic Framework Electrocatalyst FeCoNiMn-MOF on Nickel Foam.

Developing highly efficient, cost-effective, non-noble-metal-based electrocatalysts with superior performance and stability for oxygen evolution reactions is of immense challenge as well as great importance for the upcoming sustainable and green energy conversion technologies. The multivariate metal-organic frameworks with hierarchical porous structures and unsaturated coordination modes are considered to be promising emerging energy materials. In this work, a series of multimetallic MOFs were directly grown on nickel foam (NF) through the solvothermal method. Notably, the optimized tetrametallic FeCoNiMn-MOF/NF shows a low overpotential of 239 mV to achieve a current density of 50 mA cm-2 with a Tafel slope of 62.05 mV dec-1 for OER in 1 M KOH. It also exhibits excellent stability and durability over 100 h in chronoamperometric studies. The enhanced performance is closely tied to the high activity of iron and nickel ions and the decomposed and reconstructed Ni/Fe-OOH intermediates of the FeCoNiMn-MOF/NF during the OER process, which are revealed by XPS analysis and in situ Raman spectroscopy. This present work demonstrates the feasibility and advantage of utilizing highly efficient and durable multimetallic MOFs for electrocatalytic oxygen evolution.

Rational Design of Organic Electrocatalysts for Hydrogen and Oxygen Electrocatalytic Applications.

Efficient electrocatalysts are pivotal for advancing green energy conversion technologies. Organic electrocatalysts, as cost-effective alternatives to noble-metal benchmarks, have garnered attention. However, the understanding of the relationships between their properties and electrocatalytic activities remains ambiguous. Plenty of research articles regarding low-cost organic electrocatalysts started to gain momentum in 2010 and have been flourishing recently though, a review article for both entry-level and experienced researchers in this field is still lacking. This review underscores the urgent need to elucidate the structure-activity relationship and design suitable electrode structures, leveraging the unique features of organic electrocatalysts like controllability and compatibility for real-world applications. Organic electrocatalysts are classified into four groups: small molecules, oligomers, polymers, and frameworks, with specific structural and physicochemical properties serving as activity indicators. To unlock the full potential of organic electrocatalysts, five strategies are discussed: integrated structures, surface property modulation, membrane technologies, electrolyte affinity regulation, and addition of anticorrosion species, all aimed at enhancing charge efficiency, mass transfer, and long-term stability during electrocatalytic reactions. The review offers a comprehensive overview of the current state of organic electrocatalysts and their practical applications, bridging the understanding gap and paving the way for future developments of more efficient green energy conversion technologies.