Efficient Catalyst Research Articles

Nickel-doped Cobalt Phosphide with Phosphorus-vacancy-abundant as an Efficient Catalyst for Non-aqueous and Quasi-solid-state Li-O2 Batteries

Widely acknowledged as a key strategy to tackle Li-O2 battery challenges, designing electrocatalysts with superior performance is crucial. Elemental doping and vacancy engineering can modify the local electronic structure, enhancing adsorption and catalytic activity. Nickel-doped cobalt phosphide, rich in phosphorus vacancies, was synthesized to boost electrochemical efficiency in Li-O2 batteries. These nanocomposites exhibited exceptional performance in non-aqueous Li-O2 batteries, with low overpotential and remarkable cycling stability up to 741 cycles at 500 mA g-1. Additionally, with quasi-solid-state electrolytes, the batteries retained performance for 91 cycles. This study underscores the potential of elemental doping and vacancy engineering in transition-metal-phosphides for Li-O2 battery development.

Anchored silver-palladium aerogel on carbon cloth via diazonium chemistry for electrochemical reduction of CO2

Electrochemical CO2 reduction reaction (eCO2RR) is a promising route for removal of CO2 from the atmosphere and transforming it into value-added products. The development of new and efficient catalysts plays a vital role in this regard. Here a combination of carbon grafting and bimetallic metal aerogel is presented as a catalyst for eCO2RR. The grafted surface plays an essential function in assembling the catalyst on the carbon cloth (CC) surface as a supported catalyst. Herein, we describe the use of para-aminothiophenol (p-TP) as a grafting agent combined with diazonium chemistry to fix a metallic aerogel catalyst on CC as support. The silver, palladium and bi-metallic silver-palladium aerogels (Ag-p-TP, Pd-p-TP, and AgPd-p-TP) anchored onto the surface of CC yielding the corresponding surface-bound materials were used for testing the electrochemical reduction of CO2. The mono-metallic Ag carbon cloth (Ag-p-TP/CC) exhibited the ability in reducing CO2 to CO with moderate Faradaic efficiency (FE) of 74 % in 0.1 M, NaHCO3 electrolyte at pH = 7.5. The bimetallic AgPd-p-TP-CC further enhanced the Faradaic efficiency for CO formation to 88.7 %, with an unexpectedly low onset potential of −0.09 V vs. RHE. Surprisingly, formate was identified to be the liquid product when Pd-p-TP-CC and AgPd-p-TP-CC were used, with maximal FEformate of 19.0 % and 25.7 % at −1.0 V vs. RHE, respectively. In contrast, CC lacking the chemical grafting that allows immobilization of the metal aerogel (Ag-Pd/CC) exhibits lower FEco% for eCO2RR, highlighting the importance of this chemical modification of the carbon cloth surface. Diazonium chemistry coupled with metal aerogels is a new approach to generating surface-bound catalysts for the effective reduction of CO2.

Machine-Learning-Assisted Descriptors Identification for Indoor Formaldehyde Oxidation Catalysts.

The development of highly efficient catalysts for formaldehyde (HCHO) oxidation is of significant interest for the improvement of indoor air quality. Up to 400 works relating to the catalytic oxidation of HCHO have been published to date; however, their analysis for collective inference through conventional literature search is still a challenging task. A machine learning (ML) framework was presented to predict catalyst performance from experimental descriptors based on an HCHO oxidation catalysts database. MnOx, CeO2, Co3O4, TiO2, FeOx, ZrO2, Al2O3, SiO2, and carbon-based catalysts with different promoters were compiled from the literature. Notably, 20 descriptors including reaction catalyst composition, reaction conditions, and catalyst physical properties were collected for data mining (2263 data points). Furthermore, the eXtreme Gradient Boosting algorithm was employed, which successfully predicted the conversion efficiency of HCHO with an R-square value of 0.81. Shapley additive analysis suggested Pt/MnO2 and Ag/Ce-Co3O4 exhibited excellent catalytic performance of HCHO oxidation based on the analysis of the entire database. Validated by experimental tests and theoretical simulations, the key descriptor identified by ML, i.e., the first promoter, was further described as metal-support interactions. This study highlights ML as a useful tool for database establishment and the catalyst rational design strategy based on the importance of analysis between experimental descriptors and the performance of complex catalytic systems.

Effect of support structure of Pt/Silicaite-1 catalyst on non-thermal plasma (NTP) assisted chlorobenzene degradation and PCDD/Fs formation

Development of efficient catalysts for non-thermal plasma (NTP) assisted catalysis to mitigate the formation of harmful by-products is a significant challenge in the degradation of chlorinated volatile organic compounds (Cl-VOCs). In this study, catalytically active Pt nanoparticles supported on non-porous SiO2 and silicalite-1 zeolites (S1) with different pore structure were comparatively investigated for catalytic chlorobenzene degradation under NTP condition. It was shown that the pore structure could significantly impact the metal size and metal dispersion rate. Pt supported on modified S1 hierarchical meso-micro-porous silicalite-1 (Pt/D-S1) exhibited the smallest particle size (∼6.19 nm) and the highest dispersion rate (∼1.87). Additionally, Pt/D-S1 demonstrated superior catalytic performance compared to the other catalysts, achieving the highest chlorobenzene conversion and COx selectivity at about 80% and 75%, respectively. Furthermore, the pore structure also affected the formation of by-products according to the findings from GC-MS analysis. Pt/SiO2 generated a total of 18 different species of organic compounds, whereas only 12 species of organic by-products were identified in the Pt/D-S1 system (e.g. polychlorinated compounds like 3,4 dichlorophenol were exclusively identified in Pt/SiO2). Moreover, dioxin-like polychlorinated biphenyl and other chlorinated organic compounds, which have potential to form highly toxic dioxins, were detected in the catalysts. HRGC-HRMS confirmed and quantified the 17 different dioxin/furans formed on Pt/SiO2 (25,100 ng TEQ kg−1), Pt/S1 (515 ng TEQ kg−1) and Pt/D-S1 (367 ng TEQ kg−1). The correlation between synthesis-structure-performance in this study provides insights into the design of catalysts for deep oxidation of Cl-VOCs in NTP system.

Strategic regulation of nitrogen-containing intermediates for enhanced nitrate reduction over Co3O4/SiC catalyst having multiple active centers

Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction (NO3RR) is crucial for the enhancement of reaction efficiency. However, it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst. Here, a family of n%-Co3O4/SiC (n=5, 8, 12, 20) catalysts with a delicate percentage of Co2+ and Co3+ were prepared for NO3RR. We found that Co3+ primarily acts as the active site for NO3− reduction to NO2−, while Co2+ is responsible for the conversion of NO2− to NH3. Moreover, the conversion of these intermediates over the active sites is autonomous and separately controllable. Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia. Combining the experimental studies and density functional theory (DFT) calculations, it is discovered the pathway (*NHO→*NHOH→*NH2OH→*NH2→*NH3) is more favorable due to the lower ΔG value (0.25 eV) for the rate-limiting step (*NO→*NHO). The NH3 yield rate of 8%-Co3O4/SiC reached 1.08 mmol/(cm2 h) with a Faradaic efficiency of 96.4% at −0.89 V versus the reversible hydrogen electrode (RHE), surpassing those of most reported non-noble NO3RR catalysts. This strategy not only provides an efficient catalyst for NO3RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites, thereby presenting a new approach to enhance the efficiency of intricate reactions.

Promoted catalytic property of Cu/SSZ-13 by introducing a minority of Mn for NO removal from diesel engine exhaust

The Cu-exchanged SSZ-13 with the small-pore chabazite framework is considered as a highly efficient catalyst for selective catalytic reduction of NO with NH3 (NH3-SCR). In order to further improve the catalytic property, a series of Mn ion-assisted Cu/SSZ-13 powder catalysts were prepared by co-exchange method and stepwise exchange method. It is found that the NH3-SCR activity, N2 selectivity, hydrothermal stability and sulfur resistance of Cu/SSZ-13 are promoted by introducing a minority of Mn (0.15%–0.23%(mass)) through co-exchange method. Characterization results revel that the Cu,Mn co-exchange enables the higher amounts of Cu2+ active sites, the abundant medium strong and strong acid, the optimized ratio of lewis acid to Brønsted acid, etc., which are required for a good NH3-SCR catalytic property over broad temperature range and under harsh working environment. Moreover, a monolithic catalyst was prepared by impregnating a cordierite ceramic support into the coating slurry containing the optimized CuMn/SSZ-13 powder. The diesel engine bench tests show that Cu,Mn co-exchange gives the monolith catalyst a better catalytic property than commercial catalysts. This work provides an important guidance for the rational design of secondary-ion-assisted zeolites applied in NH3-SCR.

Supported of gold nanoparticles on carboxymethyl lignin modified magnetic nanoparticles as an efficient catalyst for reduction of nitroarenes and treatment of human melanoma

This article represents the synthesis and characterizations of Au NPs immobilized and carboxymethyl lignin (CML) modified Fe3O4 nanoparticles (Fe3O4@CML/Au NPs) following a bio-inspired protocol without the participation of any toxic and harmful reductant or stabilizers. Following various physicochemical methodologies, such as FT-IR, FE-SEM, TEM, EDX, XRD, VSM, and ICP-OES, the textural characteristics and different structural aspects were evaluated. The Fe3O4@CML/Au NPs nanocomposite was subsequently explored towards the catalytic reduction of diverse aromatic nitro functions using green conditions. An excellent yield were achieved within very short reaction time. Nine recycling runs of the nanocatalyst were completed without a discernible loss of catalytic activity, thanks to its easy magnetic recovery. The DPPH assay was carried out to examine the antioxidant effectiveness. The Fe3O4@CML/Au NPs nanocomposite inhibited half of the DPPH in a 250 μg/mL solution. To measure the anti-human melanoma efficacy of Fe3O4@CML/Au NPs nanocomposite, MTT assay was applied on HT144, MUM2C, IPC-298 and SKMEL24 cell lines. Fe3O4@CML/Au NPs nanocomposite had high anti-human melanoma efficacy on above tumor cells. The best finding of anti-human melanoma properties of Fe3O4@CML/Au NPs nanocomposite was seen in the case of the SKMEL24 cell line. The IC50 of Fe3O4@CML/Au NPs nanocomposite was 137, 145, 185, and 125 μg/mL against HT144, MUM2C, IPC-298 and SKMEL24 cells, respectively. This research exhibited remarkable anti-human melanoma and antioxidant efficacies of Fe3O4@CML/Au NPs nanocomposite in the in vitro condition.

Microwave Assisted Benzoin Condensation using N,N-Dimethylbenzimidazolium Iodide as an Efficient Greener Catalyst in Neutral Ionic Liquid [Bmim]BF4

The utilization of N,N-dimethylbenzimidazolium iodide as a catalyst in [Bmim]BF4 for benzoin condensation under microwave irradiation demonstrates its efficiency and eco-friendliness. This method enables the synthesis of α-hydroxy carbonyl compounds from various aromatic and heteroaromatic aldehydes with significant yields, ranging from good to high (89-96%). The reactions proceed swiftly, yielding no detectable byproducts. Moreover, the recycled reaction media, comprising benzimidazolium salt and NaOH after extraction, can be reused multiple times without a significant loss of efficiency.

Durable Ru Nanocrystal with HfO2 Modification for Acidic Overall Water Splitting.

Durable and efficient bi-functional catalyst, that is capable of both oxygen evolution reaction and hydrogen evolution reaction under acidic condition, are highly desired for the commercialization of proton exchange membrane water electrolysis. Herein, we report a robust L-Ru/HfO2 heterostructure constructed via confining crystalline Ru nanodomains by HfO2 matrix. When assembled with a proton exchange membrane, the bi-functional L-Ru/HfO2 catalyst-based electrolyzer presents a voltage of 1.57 and 1.67 V to reach 100 and 300 mA cm-2 current density, prevailing most of previously reported Ru-based materials as well as commercial Pt/C||RuO2 electrolyzer. It is revealed that the synergistic effect of HfO2 modification and small crystalline domain formation significantly alleviates the over-oxidation of Ru. More importantly, this synergistic effect facilitates a dual-site oxide path during the oxygen evolution procedure via optimization of the binding configurations of oxygenated adsorbates. As a result, the Ru active sites maintain the metallic state along with reduced energy barrier for the rate-determining step (*O→*OOH). Both of water adsorption and dissociation (Volmer step) are strengthened, while a moderate hydrogen binding is achieved to accelerate the hydrogen desorption procedure (Tafel step). Consequently, the activity and stability of acidic overall water splitting are simultaneously enhanced.

A mini review on the applications of artificial intelligence (AI) in surface chemistry and catalysis

Abstract This review critically analyzes the incorporation of artificial intelligence (AI) in surface chemistry and catalysis to emphasize the revolutionary impact of AI techniques in this field. The current review examines various studies that using AI techniques, including machine learning (ML), deep learning (DL), and neural networks (NNs), in surface chemistry and catalysis. It reviews the literature on the application of AI models in predicting adsorption behaviours, analyzing spectroscopic data, and improving catalyst screening processes. It combines both theoretical and empirical studies to provide a comprehensive synthesis of the findings. It demonstrates that AI applications have made remarkable progress in predicting the properties of nanostructured catalysts, discovering new materials for energy conversion, and developing efficient bimetallic catalysts for CO2 reduction. AI-based analyses, particularly using advanced NNs, have provided significant insights into the mechanisms and dynamics of catalytic reactions. It will be shown that AI plays a crucial role in surface chemistry and catalysis by significantly accelerating discovery and enhancing process optimization, resulting in enhanced efficiency and selectivity. This mini-review highlights the challenges of data quality, model interpretability, scalability, and ethical, and environmental concerns in AI-driven research. It highlights the importance of continued methodological advancements and responsible implementation of artificial intelligence in catalysis research.

Silk derived electrospun carbon nanofibers loaded with CoS nanoparticles as efficient hydrogen evolution reaction catalysts in acidic and alkaline media

The design of a stable and efficient hydrogen evolution catalyst across the entire pH range is of significant importance for the development of hydrogen production technology by electrocatalytic water splitting. This study chose biomass silk fibroin protein as the electrospinning raw material, synthesizing a hybrid membrane of CoS@carbon nanofibers (CNF) with a layered core–shell structure through simple carbonization and hydrothermal treatment. The CoS nanoparticles can grow uniformly and densely on the CNF. By varying the concentrations of hexahydrate cobalt nitrate (Co(NO3)2·6H2O) and thiourea (CH4N2S), the morphology of the synthesized CoS nanoparticles on CNF can be controlled. Different microscopic morphologies lead to differences in the activity of the hydrogen evolution reaction (HER), attributed to variations in the exposed active sites for different morphologies. Compared to pure CNF, the CoS-2@CNF hybrid membrane exhibits excellent HER activity in both acidic and alkaline electrolytes. This highlights the synergistic catalytic effect between CNF and CoS particles. This work provides guidance for the rational design of bio-based catalysts with excellent performance.

Theoretical insights on 3D transition metal anchored poly[5,10,15,20-tetra(4-ethynylphenyl)porphyrin]diyne as highly efficient bifunctional catalyst toward ORR and OER

Searching for highly active oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) catalysts is a challenging task in the development of clean energy devices. Herein, by using the poly[5,10,15,20-tetra(4-ethynyl-phenyl)porphyrin]diyne (TEPPD), we designed ORR and OER catalysts by anchoring 3d transition metal into TEPPD (TM@TEPPD, TM = Mn-Zn). Our study indicated that Fe@TEPPD is the best bifunctional catalyst for both ORR and OER. By proposing a proper descriptor, Ni-N3@TEPPD (Ni is only coordinated with three N atoms) is designed and also predicted to be a promising bifunctional catalyst. For Fe@TEPPD, ORR and OER become inactive when the acetylene bond in TEPPD is broken. The surface Pourbaix diagram indicated that on the surface of Fe@TEPPD, ORR and OER can be carried out at the whole pH region due to the high dissolution potential of Fe2+. For Ni-N3@TEPPD, however, the dissolution potential 0.71 V for Ni2+is low. Thus, for Ni-N3@TEPPD, ORR can be carried out only after pH>2.54, while OER is not likely at the whole pH region. This suggested that the conclusions from the free energy changes at URHE=0 and pH=0 could be different when different potentials and pH values are considered.

Organic Acid‐Assisted Preparation of Hydroxyapatite‐supported Ni Catalysts for Arene Hydrogenation

Developing non‐noble metal catalysts that can efficiently and selectively hydrogenate arenes remains a significant challenge. In this study, we developed efficient Ni catalysts for the arene hydrogenation based on an organic acid‐regulated impregnation strategy. These easily accessible Ni catalysts demonstrated exceptional efficiency, selectivity, reusability, and good substrate compatibility. The influence of carbon chain lengths and side‐chain hydroxyl or amino groups on dicarboxylic acids used in the catalyst preparation was comprehensively investigated. Characterizations and kinetic studies demonstrated the influence of organic acids on the size of Ni nanoparticles, the proportion of metallic nickel, and the strength of surface acidity. These factors influenced the activation of arene and hydrogen, thereby affecting the hydrogenative activity. Notably, hydroxyapatite‐supported Ni catalyst, assisted by tartaric acid (Ni‐TA/HAP) with an appropriate tartaric acid‐to‐nickel ratio, resulted in relatively smaller Ni nanoparticles, an increased proportion of Ni0, and more acidic sites, thereby exhibiting the best hydrogenation performance.

Steering sp‐Carbon Content in Graphdiynes for Enhanced Two‐Electron Oxygen Reduction to Hydrogen Peroxide

AbstractCompared to sp2‐hybridized graphene, graphdiynes (GDYs) composed of sp and sp2 carbon are highly promising as efficient catalysts for electrocatalytic oxygen reduction into oxygen peroxide because of the high catalytic reactivity of the electron‐rich sp‐carbon atoms. The desired catalytic capacity of GDY, such as catalytic selectivity and efficiency, can theoretically be achieved by strategically steering the sp‐carbon contents or the topological arrangement of the acetylenic linkages and aromatic bonds. Herein, we successfully tuned the electrocatalytic activity of GDYs by regulating the sp‐to‐sp2 carbon ratios with different organic monomer precursors. As the active sp‐carbon atoms possess electron‐sufficient π orbitals, they can donate electrons to the lowest unoccupied molecular orbital (LUMO) orbitals of O2 molecules and initiate subsequent O2 reduction, GDY with the high sp‐carbon content of 50 at % exhibits excellent capability of catalyzing O2 reduction into H2O2. It demonstrates exceptional H2O2 selectivity of over 95.0 % and impressive performance in practical H2O2 production, Faraday efficiency (FE) exceeding 99.0 %, and a yield of 83.3 nmol s−1 cm−2. Our work holds significant importance in effectively steering the inherent properties of GDYs by purposefully adjusting the sp‐to‐sp2 carbon ratio and highlights their immense potential for research and applications in catalysis and other fields.

Enhancing Nitrogen Reduction Reaction through Formation of 2D/2D Hybrid Heterostructures of MoS2@rGO.

Given the challenging task of constructing an efficient nitrogen reduction reaction (NRR) electrocatalyst with enhanced ambient condition performance, properties such as high specific surface area, fast electron transfer, and design of the catalyst surface constitute a group of key factors to be taken into consideration to guarantee outstanding catalytic performance and durability. Thereof, this work investigates the contribution of the 2D/2D heterojunction interface between MoS2 and reduced graphene oxide (rGO) on the electrocatalytic synthesis of NH3 in an alkaline media. The results revealed remarkable NRR performance on the MoS2@rGO 2D/2D hybrid electrocatalyst, characterized by a high NRR sensitivity (faradaic efficiency) of 34.7% with an NH3 yield rate of 3.98 ± 0.19 mg h-1 cm-2 at an overpotential of -0.3 V vs RHE in 0.1 M KOH solution. The hybrid electrocatalysts also exhibited selectivity for NH3 synthesis against the production of the hydrazine (N2H4) byproduct, hindrance of the competitive hydrogen evolution reaction (HER), and good durability over an operation period of 8 h. In hindsight, the study presented a low-cost and highly efficient catalyst design for achieving enhanced ammonia synthesis in alkaline media via the formation of defect-rich ultrathin MoS2@rGO nanostructures, consisting predominantly of an HER-hindering hexagonal 2H-MoS2 phase.

Investigation of Co3O4 modified carbon black as an efficient non-noble metal oxygen reduction catalyst in self-driven phosphorus recovery systems

Phosphorus and nitrogen recovery from urine in the form of struvite via a Mg-air fuel cell (MAFC) platform has previously been reported as a promising approach to achieving sustainable development goals. However, the applicability of this technology has been hindered by the expensive cathodic catalyst, i.e., Pt/C. In this study, an efficient and cost-effective non-precious metal catalyst, the Co3O4 doped carbon black (CB-ZIF-900), was developed to maximize nitrogen and phosphate recovery from urine while reducing investment costs. CB-ZIF-900 exhibited an oxygen reduction reaction current density of 2.95 mA cm−2 and an electron transfer number between 3.7 and 3.9 in urine solution, which approached those of commercial Pt/C at the same testing conditions. Using the MAFC, over 99 % of phosphorus was removed from urine, and >95 % of phosphorus was recovered in the precipitates. Stable phosphorus removal efficiency and precipitates composition were observed over five consecutive batch experiments. Furthermore, the MAFC with CB-ZIF-900 exhibited a maximum power density of 594.89 W m−3, surpassing that with commercial Pt/C by 9.3 %. These findings underscore the utility of the highly efficient and cost-effective CB-ZIF-900 for advancing the scalability and widespread applications of self-driven phosphorus recovery systems.

Phosphine Substituted N‐coordinated Stannylene: Efficient Catalyst in Ketone Hydroboration.

P‐substituted stannylene (Ph2PCH2)(L)Sn containing N,C,N‐chelated ligand (L = [2,6‐(Me2NCH2)2C6H3]) was prepared. Complex was further oxidized to prepare P‐substituted organotin(IV) compounds (Ph2PCH2)(L)SnX2. Finally, P(S)‐substituted N‐coordinated stannylene [(Ph2P(S)CH2](L)Sn containing P atom in the oxidation state +V was also prepared. All these P‐substituted organotins were tested as the catalysts for the hydroboration of ketones to see the effect of oxidation numbers of Sn/P atoms. Stannylene (Ph2PCH2)(L)Sn showed remarkable conversions with TOF about 1800 h‐1 and it is suitable to the reduction of several ketones. The mechanistic studies are also discussed.

UiO-67 metal-organic frameworks with dual amino/iodo functionalization, and mixed Zr/Ce clusters: Highly selective and efficient photocatalyst for CO2 transformation to methanol

Metal-organic frameworks (MOFs) are promising tools for photocatalytic CO2 reduction (PCR) to produce valuable added-value products. However, existing MOFs demonstrate significantly weaker potential for PCR to MeOH compared to fuels like CO, CHOOH, and CH4. This study address this challenge by exploring a series of bifunctional UiO-67 MOFs containing NH2 and I groups with varying Ce to Zr metal node ratios (0, 10, 20, 29, and 40 % Ce). These MOFs, denoted as Zr/CeX%-UiO-67(NH2, I), were probed for their ability to convert CO2 to MeOH under solar irradiation without the need for a photosensitizer. The results demonstrate a remarkable increase in both selectivity and efficiency for MeOH production with increasing Ce content. Notably, Zr/Ce29%-UiO-67(NH2, I) achieves 100 % selectivity for MeOH production, along with MeOH productivity of 44.7 µmolh−1g−1, significantly surpassing previously reported UiO-based MOFs for PCR-to-MeOH conversion. Furthermore, this MOF exhibits exceptional CO2 uptake capacity compared to pristine UiO-67 and many established MOFs, further highlighting its catalytic efficacy. The outstanding photocatalytic performance of Zr/Ce40%-UiO-67(NH2, I) can be attributed to a synergistic combination factors: (i) the optimal incorporation of redox-active Ce metal sites, (ii) enhanced CO2 capture facilitated by the cooperative interaction of NH2 and I groups, and (iii) the introduction of amino functions that broaden the light absorption range of the MOF. This work demonstrates a successful strategy for incorporating various functionalities into MOFs, paving the way for the design of highly selective and efficient PCR catalysts for MeOH production.

Hierarchical Porous N-Doped Carbon Particles Derived from ZIF-8 as Highly Efficient H2S Selective Oxidation Catalysts.

In the selective oxidation of H2S, the catalytic activity over N-doped carbon-based catalysts is significantly influenced by the accessibility of active sites and the mass transfer rates of reactant molecules (e.g., H2S and O2) as well as generated sulfur monomers. Therefore, it is crucial for enhancing the initial performance via the controlled synthesis of carbon-based catalysts with highly exposed active sites and unique porous structures. Herein, we reported on an efficient strategy to synthesize nanosized N-doped carbon particles with hierarchical porous structures by directly pyrolyzing an oversaturated NaCl-encapsulated ZIF-8 precursor mixture. The introduction of NaCl not only serves as a pollution-free template to promote the formation of graphitic carbon layers but also acts as an intercalating agent to guide the derivation of hierarchical porous structures, as well as enhances the amount of active nitrogen species in the catalysts. As a result, the as-prepared H-NC800 catalyst shows excellent H2S selective oxidation performance (sulfur formation rate is 794 gsulfur·kgcat-1·h-1), good stability (>80 h), and antiwater vapor properties. The characterization results and DFT calculations indicate the crucial role of pyridinic N in the adsorbing and activating reactant molecules (H2S, O2). Furthermore, nanoscale N-doped carbon particles accelerated the rapid transport of generated sulfur monomers under a hierarchical porous structure. This investigation introduces a distinctive strategy for synthesizing ZIF-8-derived N-doped carbon nanosized with a hierarchical porous structure, while its efficient and stable H2S selective oxidation performance highlights significant potential for practical implementation in the industrial desulfurization process.

Investigating the electrochemical performance of Mn3O4/MoMn2P12 mixed-phase catalyst on MWCNT for high specific energy supercapacitors and HER/OER reactions

A versatile Mn/MoMn hybrid oxide/phosphide composite (MnO/MoMnP) supported on MWCNT is synthesized using hydrothermal method and in-situ phosphorization methods. This composite serves as a catalyst for supercapacitors and oxygen and hydrogen evolution reactions (OER/HER) in electrochemical water splitting. XRD analysis confirmed the presence of mixed-phase of Mn3O4 and MoMn2P12. Electrochemical tests revealed exceptional charge storage performance for MnO/MoMnP/MWCNT, with a high specific capacitance(436 F g−1 at 1 A g−1) and impressive capacitance retention (96.51 % for 5000 cycles at 15 A g−1). This performance surpasses that of bare MnO/MoMnP by 50 %. Furthermore, we assembled a MnO/MoMnP/MWCNT//MWCNT device, that achieved a remarkable energy density of 128.11 W h kg−1 at an ultra-high-power density of 1920 W kg−1, along with excellent cycling stability (92.5 % for 5000 cycles). Moreover, the MnO/MoMnP/MWCNT composite exhibited a remarkable bifunctional electro catalytic activity for OER and HER, with low overpotentials of 335 and 430 mV at 10 mA cm−2 in 1 M KOH solution. These results highlight MnO/MoMnP/MWCNT as a promising and efficient alternative catalyst for future applications in supercapacitors and water electrolysis.