Full pH Range Research Articles

NiCoMn phosphides-based 3D nanoflowers as universal electrocatalyst towards hydrogen evolution reaction at all pH values

In addressing the pH constraints encountered in real-world electrolyte environments, it is of great practical significance to establish a universal electrocatalyst capable of facilitating the hydrogen production reaction (HER) across all pH levels. Herein, non-precious metals NiCoMn were incorporated into a nickel foam skeleton and subjected to phosphorization treatment, yielding the NiCoMn-O-P@NF catalyst suitable for HER across the entire pH spectrum. Leveraging the synergistic effects of these three metals and phosphating regulation, the synthesized NiCoMn-O-P@NF demonstrates efficient HER catalytic performance in acidic (−0.05 VRHE at 10 mA cm−2), alkaline (−0.17 VRHE at 10 mA cm−2), and neutral (−0.25 VRHE at 10 mA cm−2) electrolytes, with exceptional stability. This study presents a cost-effective electrocatalyst with robust and enduring catalytic performance for HER over the full pH range, offering an environmentally friendly solution to the challenges of practical hydrogen generation.

Electronic regulation of Ce,F-Ni2P/CoP catalyst for efficient water splitting

Designing efficient non-precious-metal bifunctional electrocatalysts is still challenging at present. Herein, the efficient Ce,F-Ni2P/CoP electrocatalyst for water splitting was successfully fabricated. As shown from the present investigation, the codoping of Ce and F in Ni2P/CoP induced the f-p-d gradient orbital coupling in the Ce-F-metal structural unit of the catalyst, significantly reducing the work function of the catalyst, which accelerated the reaction kinetics and improved the intrinsic catalytic activity. The catalyst exhibited the outstanding hydrogen evolution reaction (HER) activity in the full pH range and, especially in alkaline electrolyte, an ultra-low oxygen evolution reaction (OER) overpotential of 243 mV at 50 mA·cm−2 and an excellent HER overpotential of 88 mV at 10 mA·cm−2 were achieved. Moreover, Ce,F-Ni2P/CoP displayed an excellent overall water splitting (OWS) performance with η10 = 1.52 V. DFT theoretical calculations also showed that the gradient orbital coupling resulted in the reduction of the work function of the catalyst. Our work provides a new understanding of designing and constructing high-performance catalysts.

Anchoring gadolinium oxide nanoparticles onto CuInZnS: Efficient photocatalytic tetracycline degradation and mechanism analysis

Photocatalysis technology is one of the potential methods to remit the growing issues of environmental pollution. It is of great significance to rationally design high performance antibiotic wastewater degradation catalysts in the whole pH range. In this experiment, Gd2O3 nanoparticles (GdO NPs) were successfully grown onto CuInZnS (CIZS) by a simple hydrothermal method. The introduction of GdO has obvious effects on the nanosheet thickness of CIZS, which reduces carrier transport distances and improves the active sites number of CIZS. What’s more, the SO4•- absorption and electron transfer ability are also greatly optimized. Under 300 W Xe light, tetracycline can be efficient degraded more than 93 % in the whole pH range, which presents absolute advantage compared to CIZS and GdO. Based on the combination of experimental characterization and density functional theory calculations, the proposed photocatalytic tetracycline degradation pathway and mechanism have been given. Moreover, the results of toxicity analysis proved that the CIZS-GdO catalyst could successfully reduce the toxicity of tetracycline wastewater. This work has reference value for the application of rare earth oxides in the field of photocatalysis at full pH range.

Interface-stabilized high-valent Sn enables efficient CO2 electroreduction to formate/formic acid across the full pH range

The electrocatalytic synthesis of formate/formic acid (HCOO−/HCOOH) from CO2 can mitigate environmental issues and provide high-value-added products. Although tin oxide is an excellent catalyst for HCOO−/HCOOH production, it is easily reduced to its metallic state at high potentials, which decreases its activity. Additionally, tin oxide is challenging to stabilize in acidic electrolytes. Here, we introduced Cu to tin oxide catalysts to form Cu6Sn5@SnOx during the CO2 electroreduction process (CO2RR), achieving a high HCOO−/HCOOH Faradaic efficiency (88.4 % at 800 mA cm−2 in 1 M KOH electrolyte, 87.8 % at 300 mA cm−2 in 0.1 M H2SO4 electrolyte containing 1 M K+) and a maximum HCOO− partial current density (757.5 mA cm−2). The in situ spectroscopy and DFT calculations results revealed that the SnOx/Cu6Sn5 alloy interface plays a crucial role in stabilizing the surface high-valent Sn, which provides a thermodynamically stable environment for adsorbed *OCHO intermediate. This discovery offers new insights into the roles of each component in bimetallic catalysts in CO2 reduction.

Myrica rubra-like P–Co1-xS/C as an efficient catalyst for all-pH hydrogen evolution reaction

The development of cheap, efficient and stable hydrogen-producing catalysts is the current research focus, especially the catalysts that can work stably in the whole pH range. In this work, a myrica rubra-like structure of P–Co1-xS/C was synthesized by hydrothermal reaction, sulfurization and phosphorization using spherical flower-like cobalt glycerate (CoG) as precursor. The design of this multilevel structure of P–Co1-xS/C effectively increases the specific surface area. The doping phosphorus and the protection of carbon layer greatly improve catalytic performance and enhance the stability of Co1-xS in the hydrogen evolution reaction (HER) at full pH range. When the current density is 10 mA cm−2, the HER overpotentials of P–Co1-xS/C in acidic, alkaline and neutral solutions are 86, 93 and 167 mV, and respectively. The Tafel slopes of P–Co1-xS/C in acidic, alkaline and neutral solutions are 82, 100 and 103 mV dec−1, respectively. In addition, the electrocatalyst also displays excellent electrochemical long-term stability. After 2000 cycles or 20 h long-term testing, its catalytic activity remains stable without obvious decrease at full pH range.

Multi-Scale Development and Integration of Granular Activated Carbon Electrodes in Multiphase Electrochemical Systems

Providing clean water remains a significant challenge in underserved areas that lack access to public water systems or are affected by extreme natural events like hurricanes. Electrochemical technologies show promise for developing affordable and effective water treatment systems due to their ability to efficiently oxidize contaminants. Particularly, the electrochemical synthesis of in-situ reagents, such as H2O2, systems can oxidize contaminants over the full range of pH with high oxidation potential, leaving only water and oxygen at the end of process, making it a safe and effective method for water treatment. This study is focused on integrating carbon-based electrodes into electrochemical water treatment systems emphasizing their scalability, cost effectiveness, and the efficient generation of reactive oxygen species (ROS). By employing multiscale computational approaches, we develop a comprehensive mechanistic understanding and optimization of ROS generation at the surface of granular activated carbon (GAC) electrodes. Using reactive molecular dynamics simulations, the thermodynamic and transport properties of water-based electrolyte (e.g., adsorption, viscosity, and diffusion) are investigated as a function of the GAC particle size and chemistry. The obtained results show that tuning the GAC particle structure at nanoscale can improve the local diffusion rates by three times. Subsequently, multiphase continuum simulations are used to integrate the GAC electrodes in full electrochemical systems through optimizing the dispersion and the solid-liquid-gas interactions in a reactive environment. The computational findings reveal that higher production of H2O2 and are observed at optimized electrode porosity values when the GAC electrodes are integrated at the system level. These observations are linked to the complex reactive solid-fluid interactions. Specifically, the electrochemical oxygen bubble splitting and coalescence are minimized by optimizing the electrode porosity, which improves the dispersion mass transfer processes by at least one order of magnitude. This leads to higher generation rates of ROS and enhanced degradation of water contaminants. These mechanistic observations will help in designing and scaling up carbon-based electrodes for developing efficient and cost-effective electrochemical water treatment reactors.

Effect of incubation conditions of cellulase hydrolysis on mechanical pulp fibre morphology

The mechanical pulp industry is diversifying through the manufacture of high-value paper products, such as microfibrillated cellulose. However, the development of fibre quality is still energy-intensive. Enzymatic hydrolysis is hypothesized to promote fibre cutting, greater fibrillation, and reduce refining energy costs. Despite potential benefits, there is little understanding of the mechanisms behind fibre development during enzymatic hydrolysis of mechanical pulp. This work investigates how incubation pH and temperature during enzymatic hydrolysis impact the refining of mechanical pulp short fibres. Incubation with endoglucanase at pH 5 and 60 °C increased fibre cutting by approximately 20 %. Fibrillation was negatively affected at this condition, resulting in increased slim fines formation with refining. Incubation at pH 8 and 80 °C promoted >15 % reduction in fibre length, despite such conditions being associated with low enzyme activity. The pH variation modified the sedimentation height of the fibres and the conductivity of suspensions, indicating a change in fibre surface charge. Fibre morphology changes were induced by enzyme hydrolysis conducted at conditions representative of the full range of pH and temperature observed in mechanical pulp mills.

Rapid Synthesis of Nickel Hydroxide/Pt-Based Alloy Heterointerface for Hydrogen Evolution in Full pH Range.

The huge application potential of nanoelectrocatalysts can become available only under the condition of scalable and reproducible preparation of nanomaterials (NMs). It is easily overlooked that most of the preparation methods for efficient platinum (Pt)-based electrocatalysts are complicated in process and time-/energy-consuming, which is not conducive to scalable and sustainable production. Herein, we propose a rapid and facile method to in situ construct a heterointerface between nickel hydroxide (Ni(OH)2) and NiPt alloy, in which the preparation steps are easy-to-operate and can be finished in 1 h. Furthermore, the ensemble effect between the Ni(OH)2 substrate and NiPt active sites benefits the water dissociation process in nonacidic conditions, while the electronic effect in NiPt contributes to the downshifted d-band center of Pt and the proper Gibbs free energy of hydrogen species. As a result, the well-designed and quickly constructed Ni(OH)2-Ni3Pt heterointerfaces reveal lower overpotentials for HER compared with most reported Pt-based and commercial Pt/C catalysts in nonacidic conditions. This study is expected to provide useful reference information for the development of facile and robust methods for the preparation of more efficient Pt-based electrocatalysts.

Al-water reaction generates metastable aluminum cluster ions and their use in advanced oxidation processes

Our previous work indicated that hydroxyl radicals (HO•) exist in the filtrate of Al + acid + H2O2 system. In this work, the behind mechanism was investigated in detail and a new catalyst for advanced oxidation processes (AOPs) was found for the first time. It was revealed that metastable hexacoordinated aluminum cluster ions ([Al(H2O)63+]*), which are produced by Al-water reaction, can be as direct catalyst and decompose H2O2 into HO• in a full pH range (2.5–12.0), and efficiently degrade and mineralize organic pollutants without precipitates. Of course, their catalytic activity in acidic aqueous solution is higher than that in neutral and alkaline solutions. Furthermore, [Al(H2O)63+]* cluster ions have an excellent recyclability and their catalytic efficiency for generating HO• and degrading phenol and bisphenol A (BPA) did not decrease significantly even the cycling number was up to ten. Meanwhile, [Al(H2O)63+]* cluster ions have a long lifetime and can keep their catalytic activity for more than three months under ambient condition. The present finding shows that Al3+ ions can be also as a cost-efficient catalyst for AOP technology.

Engineering pH-sensitive dissolution of lipid-polymer nanoparticles by Eudragit integration impacts plasmid DNA (pDNA) transfection

Lipid-polymer nanoparticles offer a promising strategy for improving gene nanomedicines by combining the benefits of biocompatibility and stability associated with the individual systems. However, research to date has focused on poly-lactic-co-glycolic acid (PLGA) and resulted in inefficient transfection. In this study, biocompatible Eudragit constructs E100 and RS100 were formulated as lipid-polymer nanoparticles loaded with pDNA expressing red fluorescent protein (RFP) as a model therapeutic. Using a facile nanoprecipitation technique, a core–shell structure stabilised by lipid-polyethylene glycol (PEG) surfactant was produced and displayed resistance to ultracentrifugation. Both cationic polymers E100 (pH-sensitive dissolution at 5) and RS100 (pH-insensitive dissolution) produced 150–200 nm sized particles with a small positive surface charge (+3–5 mV) and high pDNA encapsulation efficiencies (EE) of 75–90%. The dissolution properties of the Eudragit polymers significantly impacted the biological performance in human embryonic kidney cells (HEK293T). Nanoparticles composed of polymer RS100 resulted in consistently high cell viability (80–100%), whereas polymer E100 demonstrated dose-dependent behaviour (20–90% cell viability). The low dissolution of polymer RS100 over the full pH range and the resulting nanoparticles failed to induce RFP expression in HEK293T cells. In contrast, polymer E100-constructed nanoparticles resulted in reproducible and gradually increasing RFP expression of 26–42% at 48–72 h. Intraperitoneal (IP) injection of the polymer E100-based nanoparticles in C57BL/6 mice resulted in targeted RFP expression in mouse testes with favourable biocompatibility one-week post-administration. These findings predicate Eudragit based lipid-polymer nanoparticles as a novel and effective carrier for nucleic acids, which could facilitate pre-clinical evaluation and translation of gene nanomedicines.

Understanding Sorption of Aqueous Electrolytes in Porous Carbon by NMR Spectroscopy.

Ion adsorption at solid-water interfaces is crucial for many electrochemical processes involving aqueous electrolytes including energy storage, electrochemical separations, and electrocatalysis. However, the impact of the hydronium (H3O+) and hydroxide (OH-) ions on the ion adsorption and surface charge distributions remains poorly understood. Many fundamental studies of supercapacitors focus on non-aqueous electrolytes to avoid addressing the role of functional groups and electrolyte pH in altering ion uptake. Achieving microscopic level characterization of interfacial mixed ion adsorption is particularly challenging due to the complex ion dynamics, disordered structures, and hierarchical porosity of the carbon electrodes. This work addresses these challenges starting with pH measurements to quantify the adsorbed H3O+ concentrations, which reveal the basic nature of the activated carbon YP-50F commonly used in supercapacitors. Solid-state NMR spectroscopy is used to study the uptake of lithium bis(trifluoromethanesulfonyl)-imide (LiTFSI) aqueous electrolyte in the YP-50F carbon across the full pH range. The NMR data analysis highlights the importance of including the fast ion-exchange processes for accurate quantification of the adsorbed ions. Under acidic conditions, more TFSI- ions are adsorbed in the carbon pores than Li+ ions, with charge compensation also occurring via H3O+ adsorption. Under neutral and basic conditions, when the carbon's surface charge is close to zero, the Li+ and TFSI- ions exhibit similar but lower affinities toward the carbon pores. Our experimental approach and evidence of H3O+ uptake in pores provide a methodology to relate the local structure to the function and performance in a wide range of materials for energy applications and beyond.

Hydrogen spillover in Pt/Ni(OH)2/Mo2TiC2Tx electrocatalyst improves pH-universal hydrogen evolution reaction

Electrocatalytic hydrogen evolution reaction (HER) shows potential to transition from fossil fuels to green renewable energy. Designed for high efficiency and stability electrocatalyst in pH-universal electrolyte is of great significance but challenging. Herein, a novel electrocatalyst of two-dimensional (2D) Mo2TiC2Tx MXene supported Pt/Ni(OH)2 (denoted as Pt/Ni(OH)2/Mo2TiC2Tx) is reported by hydrogen spillover effect for efficient HER in the full-pH range. The operando electrochemical characterization reveals that the hydrogen spillover phenomenon interactions between multi-functional catalytic sites, e.g. Pt, Ni(OH)2 and Mo2TiC2Tx, are used to enhance HER performance and expedite HER kinetics. Moreover, theoretical calculation via density functional theory demonstrates the Pt/Ni(OH)2/Mo2TiC2Tx possess free energy of absorbed hydrogen close to zero (≈– 0.09 eV), which leads to optimal activity. As expected, the electrocatalyst necessitates the overpotential of 25, 33 and 36 mV at 10 mA cm−2 in acidic, alkaline, and neutral conditions, respectively, which are outperforming Pt/C. This work furtherly demonstrates a new way to design a powerful electrocatalyst for pH-universal HER based hydrogen spillover phenomenon.

Porous MoP2/MoS2 hierarchical nanowires for efficient hydrogen evolution reaction in full pH range

Rational designing Mo-based heterojunction catalysts as hydrogen evolution catalysts is seriously significant for the widespread utilization of hydrogen energy. Here, the ingenious hierarchical construction of MoP2/MoS2 nanowires was delivered with high conductivity of porous MoP2 and abundant active sites of defect-rich MoS2. Under synergistic effect of two materials, this catalyst achieves a dramatically optimized electronic structure to boost hydrogen evolution in all-pH range. The optimal MoP2/MoS2/CC nanoreactor showed overpotentials of 47.11, 60.16, and 89.83 mV to drive −10 mA cm−2 and Tafel slopes of 51.69, 52.04, and 73.79 mV dec−1 in acidic, alkaline, and neutral media, respectively. This finding may provide an effective approach for elevating the pH-universal electrocatalytic performance in order to achieve industrial hydrogen evolution.

Amorphous RuPd bimetallene for hydrogen evolution reaction in acidic and alkaline conditions: a first-principles study.

Metallene materials can provide a large number of active catalytic sites for the efficient use of noble metals as catalysts for hydrogen evolution reaction (HER), whereas the intrinsic activity on the surface is insufficient in crystal phase. The amorphous phase with an inherent long-range disorder can offer a rich coordinate environment and charge polarization on the surface is proposed for promoting the intrinsic catalytic activity on the surface of noble metals. Herein, we designed an amorphous RuPd (am-RuPd) structure by the first principles molecular dynamics method. The performance of the acidic HER on am-RuPd can have a huge enhancement due to the free energy change of hydrogen adsorption close to zero. In alkaline conditions, the H2O dissociation energy barrier on am-RuPd is just 0.49 eV, and it is predicted that the alkaline HER performance of am-RuPd will largely exceed that of Pt nanocrystalline sheets. This work provides a strategy for enhancing the intrinsic catalytic activity on the surface and a way to design an efficient HER catalyst based on metallene materials used in both acidic and alkaline conditions.

Robust imidazole-linked Ni-phthalocyanine-based covalent-organic framework for CO2 electroreduction in the full pH range

Ni-phthalocyanine-based covalent-organic framework linked by imidazole group exhibits brilliant stability and high activity of CO2 electroreduction reaction with over 90% CO Faradic efficiency in full pH range.

Surfaces of Atmospheric Droplet Models Probed with Synchrotron XPS on a Liquid Microjet.

ConspectusThe atmosphere is a key part of the earth system comprising myriad chemical species in all basic forms of matter. Ubiquitous nano- and microscopic aerosol particles and cloud droplets suspended in the air play crucial roles in earth's climate and the formation of air pollution. Surfaces are a prominent part of aerosols and droplets, due to the high surface area to bulk volume ratios, but very little is known about their specific properties. Many atmospheric compounds are surface-active, leading to enhanced surface concentrations in aqueous solutions. Their distribution between the surface and bulk may determine heterogeneous chemistry and many other properties of aerosol and cloud droplets, but has not been directly observed.We used X-ray photoelectron spectroscopy (XPS) to obtain direct molecular-level information on the surface composition and structure of aqueous solutions of surface-active organics as model systems for atmospheric aerosol and cloud droplets. XPS is a vacuum-based technique enabled for volatile aqueous organic samples by the application of a high-speed liquid microjet. In combination with brilliant synchrotron X-rays, the chemical specificity of XPS allows distinction between elements in different chemical states and positions within molecular structures. We used core-level C 1s and N 1s signals to identify the alkyl and hydrophilic groups of atmospheric carboxylic acids, alkyl-amines, and their conjugate acids and bases. From this, we infer changes in the orientation of surface-adsorbed species and quantify their relative abundances in the surface. XPS-derived surface enrichments of the organics follow trends expected from their surface activities and we observed a preferential orientation at the surface with the hydrophobic alkyl chains pointing increasingly outward from the solution at higher concentrations. This provides a first direct experimental observation of well-established concepts of surface adsorption and confirms the soundness of the method.We mapped relative abundances of conjugate acid-base pairs in the aqueous solution surfaces from the respective intensities of distinctive XPS signals. For each pair, the protonation equilibrium was significantly shifted toward the neutral form in the surface, compared to the bulk solution, across the full pH range. This represents an apparent shift of the pKa in the surface, which may be toward either higher or lower pH, depending on whether the acid or base form of the pair is the neutral species. The surface shifts are broadly consistent with the relative differences in surface enrichment of the individual acid and base conjugates in binary aqueous solutions, with additional contributions from nonideal interactions in the surface. In aqueous mixtures of surface-active carboxylate anions with ammonium salts at near-neutral pH, we found that the conjugate carboxylic acids were further strongly enhanced. This occurs as the coadsorption of weakly basic carboxylate anions and weakly acidic ammonium cations forms ion-pair surface layers with strongly enhanced local abundances, increasing the probability of net proton transfer according to Le Chatelier's principle. The effect is stronger when the evaporation of ammonia from the surface further contributes to irreversibly perturb the protonation equilibrium, leaving a surplus of carboxylic acid. These surface-specific effects may profoundly influence atmospheric chemistry mediated by aqueous aerosols and cloud droplets but are currently not taken into account in atmospheric models.

Robust Ru-VO2 Bifunctional Catalysts for All-pH Overall Water Splitting.

Designing robust bifunctional catalysts for oxygen evolution reaction (OER) and hydrogen evolution reaction in all-pH conditions for overall water splitting (OWS) is an effective way to achieve sustainable development. Herein, a composite Ru-VO2 containing Ru-doped VO2 and Ru nanoparticles (NPs) is synthesized, and it shows a high OWS performance in full-pH range due to their synergist effect. In particular, the OER mass activities of Ru-VO2 at 1.53 V (vs RHE) in acidic, alkaline, and PBS solutions are ≈65, 36, and 235 times of commercial RuO2 in the same conditions. The "Ru-VO2 || Ru-VO2 " two-electrode electrolyzer only needs a voltage of 1.515 V (at 10 mA cm-2 ) in acidic water splitting, which can operate stably for 125 h at 10 mA cm-2 without significant voltage decay. In situ Raman spectra and in situ differential electrochemical mass spectrometry prove that the OER of Ru-VO2 in acid follows the adsorption evolution mechanism. Density functional theory calculations further reveal the synergistic effect between Ru NP and Ru-doped VO2 , which breaks the hydrogen bond network formed by *OH adsorbed on the Ru single-atom site, and thereby significantly enhances the OER activity. This work provides new insights into the design of novel bifunctional pH-universal catalysts for OWS.

Hollow-Structured and Polyhedron-Shaped High Entropy Oxide toward Highly Active and Robust Oxygen Evolution Reaction in a Full pH Range.

High entropy metal oxides (HEO) are superior to many reactions involving multi-step elementary reactions. However, controlled synthesis of hollow-structured HEO catalysts, which offers large surface area and fast mass transfer kinetics, remains challenging and unexplored due to the complicated metal precursors. Herein, a metal organic framework-templated synthesis of hollow-structured and polyhedron-shaped HEO catalysts assembled with ultra-small nanoparticles, with up to ten metal elements, can be achieved, by taking advantage of the ion-exchange method. ZnFeNiCuCoRu-O HEO catalyst displays excellent activity and ultra-stability for oxygen evolution reaction in full pH range, with an overpotential of 170 mV at a current density of 10 mA cm-2 , a Tafel slope of 56 mV dec-1 , and a decay of activity by 7% in 30 h in alkaline medium, as well as a 12% and 8% decay in acidic and neutral medium, respectively. DFT calculation indicates that the energy barrier of the potential determining step on Ru-Fe bridge site is significantly lower than any other Ru-related bridge sites for the unique hollow structured HEO structures. This work highlights the importance of ion-exchange method in preparing highly stable and active hollow-structured HEOs catalysts toward highly efficient energy conversion and storage devices.

Acid groups decorated bimetal-organic catalyst for advanced oxidation technology at full pH range

As a wastewater treatment technology, the activity of advanced oxidation process (AOPs) is strongly dependent on pH value. Herein, considering the low activity of AOPs under alkaline conditions, the acid organic ligand (nitrilotriacetic acid, NTA) was chosen to design Co-NTA metal-organic catalyst for efficient photo-Fenton reaction at full pH range. The experimental results indicate the acid ligands in Co-NTA offers more·OH that can achieve high activity under alkaline conditions. To further enhance the electron injection ability and redox cycles of Co(II)/Co(III), Ferrocene (Fc) nanoparticles was introduced to form bimetallic organic catalyst Fc-Co-NTA. The mechanism study indicates that the synergistic effect between Co-NTA and Fc promotes the activation of potassium persulfate and improves the stability of the catalyst under extreme pH conditions, while the π-π interaction between TC and Fc-Co-NTA can improve the electron injection capability and accelerate the production of·OH/SO4•-, so as to accelerate the redox cycles of Fe(II)/Fe(III) and Co(II)/Co(III), bringing about prolonged carrier lifetime and better photocatalytic activity. The possible degradation pathway of TC was investigated by Fukui function and LC-MS. A machine learning model is used to optimize the synthesis and photocatalytic parameters of Fc-Co-NTA. This study provides a new design idea to prepare highly efficient and stable photo-Fenton advanced oxidation technology at full pH range.

Ultrasmall RuM (Mo, W, Cr) Decorated on Nitrogen-doped Carbon Nanosheet with Strong Metal-support Interactions for Electrocatalytic Hydrogen Generation in Wide pH Range

Developing efficient electrocatalysts for hydrogen evolution reaction (HER) in full pH range can promote the practical applications of hydrogen energy. In this work, nitrogen doped carbon nanosheets supported RuM (Mo, W, Cr) (RuM/NCN) are prepared through an ultrafast microwave approach. The carbon nanosheet structure coupled with the ultrasmall RuM nanoparticles can expose rich active sites to optimize the catalytic activity. Moreover, the strong metal-support interactions also favor to accelerate the reactions kinetics and improve stability. Thus, the developed RuMo/NCN (RuW/NCN) show excellent HER catalytic activities with overpotentials of 72 (75) mV, 82 (82) mV and 124 (119) mV to reach current density of 10 mA cm -2 in 1 M KOH, 0.5 M H2SO4 and alkaline seawater, respectively, and also achieve excellent performance in 1 M PBS. This work provides a valid and novel avenue to design efficient electrocatalysts in renewable energy-related fields.