Higher Mass Activity Research Articles

S-doped carbon anchoring PtCo intermetallic nanoparticles for efficient proton exchange membrane fuel cells based on molecularly engineered design

Enhanced ordered intermetallic compounds excel in catalyzing the oxygen reduction reaction (ORR). We introduce a novel synthesis strategy based on molecularly engineered to address challenges in high-temperature annealing. It involves the synthesis of carbon platforms with rich edge sites, which serve as effective anchoring points for nanoparticles. By utilizing sulfur anchoring, we synthesize ordered Pt–Co intermetallic with Pt-rich shells (o-PtCo@Pt) that exhibit remarkable ORR performance. Ordered arrangement of Pt–Co endows Pt-shell with compression stress and enhances the oxidation resistance of Pt/Co sites. O–PtCo@Pt exhibits high mass activity (MA, 0.53 A mgPt−1) and specific activity (SA, 1.17 mA cm−2). It exhibits remarkable as cathodic catalyst in proton exchange membrane fuel cells. It achieves power density of 1.14 W cm−2 at 2.0 A cm−2, with MA of 0.50 A mgPt−1 at 0.9 V. It maintains stability with only 8 % power density loss after 30,000 cycles, retaining MA of 0.35 A mgPt−1.

PdSnW Ternary Alloy Nanoparticle with Excellent CO Anti‐Poisoning Activity for Boosting Alkaline Ethanol Oxidation Reaction

AbstractEfficient ethanol oxidation reaction (EOR) catalysts with anti‐poisoning ability and high selectivity are in high demand for the widespread application of direct ethanol fuel cells (DEFCs). Here, the PdSnW ternary alloy nanoparticles are synthesized by a facile solvothermal method and exhibit an enhanced EOR catalytic performance. CO stripping experiment, X‐ray photoelectron spectroscopy and in situ Fourier transform infrared are employed to study the correlation between catalyst structure and EOR catalytic performance. The oxyphilic Sn and W not only provide dangling O−H bond, accelerating the subsequent oxidation of adsorbed intermediate CO species, but also moderate the electron state of Pd, enhancing the adsorption of CH3CH2OH, thus resulting in the promotion of C−C bond cleavage and an increased C1 selectivity. As a consequence, PdSnW alloy nanoparticle catalyst exhibit a better stability and a higher mass activity than those of Pd/C, PdSn and PdW, respectively. This work not only offers novel insights to strategically design highly efficient electrocatalysts for ethanol oxidation, but also further clarifies the inherent structure‐activity relationship.

Dilute RuCo Alloy Synergizing Single Ru and Co Atoms as Efficient and CO‐Resistant Anode Catalyst for Anion Exchange Membrane Fuel Cells

AbstractRuthenium (Ru) is considered a promising candidate catalyst for alkaline hydroxide oxidation reaction (HOR) due to its hydrogen binding energy (HBE) like that of platinum (Pt) and its much higher oxygenophilicity than that of Pt. However, Ru still suffers from insufficient intrinsic activity and CO resistance, which hinders its widespread use in anion exchange membrane fuel cells (AEMFCs). Here, we report a hybrid catalyst (RuCo)NC+SAs/N‐CNT consisting of dilute RuCo alloy nanoparticles and atomically single Ru and Co atoms on N‐doped carbon nanotubes The catalyst exhibits a state‐of‐the‐art activity with a high mass activity of 7.35 A mgRu−1. More importantly, when (RuCo)NC+SAs/N‐CNT is used as an anode catalyst for AEMFCs, its peak power density reaches 1.98 W cm−2, which is one of the best AEMFCs properties of noble metal‐based catalysts at present. Moreover, (RuCo)NC+SAs/N‐CNT has superior long‐time stability and CO resistance. The experimental and density functional theory (DFT) results demonstrate that the dilute alloying and monodecentralization of the exotic element Co greatly modulates the electronic structure of the host element Ru, thus optimizing the adsorption of H and OH and promoting the oxidation of CO on the catalyst surface, and then stimulates alkaline HOR activity and CO tolerance of the catalyst.

Dilute RuCo Alloy Synergizing Single Ru and Co Atoms as Efficient and CO-Resistant Anode Catalyst for Anion Exchange Membrane Fuel Cells.

Ruthenium (Ru) is considered a promising candidate catalyst for alkaline hydroxide oxidation reaction (HOR) due to its hydrogen binding energy (HBE) like that of platinum (Pt) and its much higher oxygenophilicity than that of Pt. However, Ru still suffers from insufficient intrinsic activity and CO resistance, which hinders its widespread use in anion exchange membrane fuel cells (AEMFCs). Here, we report a hybrid catalyst (RuCo)NC+SAs/N-CNT consisting of dilute RuCo alloy nanoparticles and atomically single Ru and Co atoms on N-doped carbon nanotubes The catalyst exhibits a state-of-the-art activity with a high mass activity of 7.35 A mgRu -1. More importantly, when (RuCo)NC+SAs/N-CNT is used as an anode catalyst for AEMFCs, its peak power density reaches 1.98 W cm-2, which is one of the best AEMFCs properties of noble metal-based catalysts at present. Moreover, (RuCo)NC+SAs/N-CNT has superior long-time stability and CO resistance. The experimental and density functional theory (DFT) results demonstrate that the dilute alloying and monodecentralization of the exotic element Co greatly modulates the electronic structure of the host element Ru, thus optimizing the adsorption of H and OH and promoting the oxidation of CO on the catalyst surface, and then stimulates alkaline HOR activity and CO tolerance of the catalyst.

Exploring the synergistic role of electron-rich Pd and electron-deficient Ni in promoting electrocatalytic hydrodechlorination

Pd has been widely used in electrocatalytic hydrodechlorination (EHDC) due to its excellent catalytic properties, but the expensive price limits its large-scale application. To address the above issues, Pd/NiFeP-Ti3C2Tx/NF electrodes with excellent EHDC capability are prepared by introducing the electron-rich Pd and the electron-deficient Ni. The synergistic role of electron-rich Pd and electron-deficient Ni lowers the energy barrier for active hydrogen (H*) generation by water splitting, thus endowing Pd/NiFeP-Ti3C2Tx/NF electrodes excellent ability to generate H*. H* has the lowest migration barrier between Pd and Ni, thus Pd and Ni produce large amounts of H* that can freely migrate to attack adsorbed chlorinated pollutants. Compared to other catalysts, Pd/NiFeP-Ti3C2Tx/NF electrode has the highest mass activity and can remove various emerging chlorinated pharmaceuticals and personal care products (PPCPs). This is a novel strategy to prepare low-cost electrodes with excellent performance to facilitate the practical application of EHDC technology.

Pt1.8Pd0.2CuGa Intermetallic Nanocatalysts with Enhanced Methanol Oxidation Performance for Efficient Hybrid Seawater Electrolysis.

Seawater electrolysis is a potentially cost-effective approach to green hydrogen production, but it currently faces substantial challenges for its high energy consumption and the interference of chlorine evolution reaction (ClER). Replacing the energy-demanding oxygen evolution reaction with methanol oxidation reaction (MOR) represents a promising alternative, as MOR occurs at a significantly low anodic potential, which cannot only reduce the voltage needed for electrolysis but also completely circumvents ClER. To this end, developing high-performance MOR catalysts is a key. Herein, a novel quaternary Pt1.8Pd0.2CuGa/C intermetallic nanoparticle (i-NP) catalyst is reported, which shows a high mass activity (11.13 A mgPGM -1), a large specific activity (18.13mA cmPGM -2), and outstanding stability toward alkaline MOR. Advanced characterization and density functional theory calculations reveal that the introduction of atomically distributed Pd in Pt2CuGa intermetallic markedly promotes the oxidation of key reaction intermediates by enriching electron concentration around Pt sites, resulting in weak adsorption of carbon-containing intermediates and favorable adsorption of synergistic OH- groups near Pd sites. MOR-assisted seawater electrolysis is demonstrated, which continuously operates under 1.23V for 240h in simulated seawater and 120h in natural seawater without notable degradation.

Breaking Highly Ordered PtPbBi Intermetallic with Disordered Amorphous Phase for Boosting Electrocatalytic Hydrogen Evolution and Alcohol Oxidation.

Constructing amorphous/intermetallic (A/IMC) heterophase structures by breaking the highly ordered IMC phase with disordered amorphous phase is an effective way to improve the electrocatalytic performance of noble metal-based IMC electrocatalysts because of the optimized electronic structure and abundant heterophase boundaries as active sites. In this study, we report the synthesis of ultrathin A/IMC PtPbBi nanosheets (NSs) for boosting hydrogen evolution reaction (HER) and alcohol oxidation reactions. The resulting A/IMC PtPbBi NSs exhibit a remarkably low overpotential of only 25 mV at 10 mA cm-2 for the HER in an acidic electrolyte, together with outstanding stability for 100 h. In addition, the PtPbBi NSs show high mass activities for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR), which are 13.2 and 14.5 times higher than those of commercial Pt/C, respectively. Density functional theory calculations demonstrate that the synergistic effect of amorphous/intermetallic components and multimetallic composition facilitate the electron transfer from the catalyst to key intermediates, thus improving the catalytic activity of MOR. This work establishes a novel pathway for the synthesis of heterophase two-dimensional nanomaterials with high electrocatalytic performance across a wide range of electrochemical applications.

Breaking Highly Ordered PtPbBi Intermetallic with Disordered Amorphous Phase for Boosting Electrocatalytic Hydrogen Evolution and Alcohol Oxidation

AbstractConstructing amorphous/intermetallic (A/IMC) heterophase structures by breaking the highly ordered IMC phase with disordered amorphous phase is an effective way to improve the electrocatalytic performance of noble metal‐based IMC electrocatalysts because of the optimized electronic structure and abundant heterophase boundaries as active sites. In this study, we report the synthesis of ultrathin A/IMC PtPbBi nanosheets (NSs) for boosting hydrogen evolution reaction (HER) and alcohol oxidation reactions. The resulting A/IMC PtPbBi NSs exhibit a remarkably low overpotential of only 25 mV at 10 mA cm−2 for the HER in an acidic electrolyte, together with outstanding stability for 100 h. In addition, the PtPbBi NSs show high mass activities for methanol oxidation reaction (MOR) and ethanol oxidation reaction (EOR), which are 13.2 and 14.5 times higher than those of commercial Pt/C, respectively. Density functional theory calculations demonstrate that the synergistic effect of amorphous/intermetallic components and multimetallic composition facilitate the electron transfer from the catalyst to key intermediates, thus improving the catalytic activity of MOR. This work establishes a novel pathway for the synthesis of heterophase two‐dimensional nanomaterials with high electrocatalytic performance across a wide range of electrochemical applications.

Metal-support interface engineering for stable and enhanced hydrogen evolution reaction

Hydrogen has emerged as a green and sustainable pathway towards achieving global decarbonization and net-zero emissions, intensely driving the need for efficient hydrogen production protocols. Electrocatalytic hydrogen evolution reaction (HER) holds great potential as a scalable, eco-friendly and safe avenue for efficient hydrogen production. However, the large-scale implementation of electrocatalytic HER is substantially challenged by the high-cost and unstable materials that are mainly fabricated from noble metals, e.g., Pt and Pd. Given this challenge, we adopted an interface engineering strategy to immobilize nanoscale Pt particles within the framework of nitrogen-doped CNTs, namely Pt@N-CNTs, where electronic metal-support interaction (EMSI) plays an important role in enabling orbital rehybridization and regulating the charge transfer through the metal-support interface, thereby considerably improving the electrocatalytic activity. With limited content of noble metals, our developed Pt@N-CNTs delivered superior HER performance with an ultralow overpotential of 5.8 mV at 10 mA cm−2 and demonstrated a high mass activity of 12.72 A mgPt−1 at an overpotential of 50 mV as well as excellent stability under harsh acidic conditions. At 500 mA cm−2, Pt@N-CNTs surprisingly exhibited an overpotential of 55.2 mV, outperforming that of commercial 20 wt% Pt/C catalysts (131.5 mV). Importantly, we established a straightforward, scalable, and time-saving microwave reduction strategy, alluding to its promising commercial viability. This work therefore sheds light on the development of high-performance electrocatalysts for hydrogen evolution and water electrolysis.

Viologen-Cucurbit[7]uril Based Polyrotaxanated Covalent Organic Networks: A Metal Free Electrocatalyst for Oxygen Evolution Reaction.

Viologen-based covalent organic networks represent a burgeoning class of materials distinguished by their captivating properties. Here, supramolecular chemistry is harnessed to fabricate polyrotaxanated ionic covalent organic polymers (iCOP) through a Schiff-base condensation reaction under solvothermal conditions. The reaction between 1,1'-bis(4-aminophenyl)-[4,4'-bipyridine]-1,1'-diium dichloride (DPV-NH2) and 1,3,5-triformylphloroglucinol (TPG) in various solvents yields an iCOP-1 and iCOP-2. Likewise, employing cucurbit[7]uril (CB[7]) in the reaction yielded polyrotaxanated iCOPs, denoted as iCOP-CB[7]-1 and iCOP-CB[7]-2. All four iCOPs exhibit exceptional stability under the acidic and basic conditions. iCOP-CB[7]-2 displays outstanding electrocatalytic Oxygen Evolution Reaction (OER) performance, demanding an overpotential of 296 and 332mV at 10 and 20mA cm-2, respectively. Moreover, the CB[7] integrated iCOP-2 exhibits a long-term stable nature for 30h in 1m KOH environment. Further, intrinsic activity studies like TOF show a 4.2-fold increase in generation of oxygen (O2) molecules than the bare iCOP-2. Also, it is found that iCOP-CB[7]-2 exhibits a high specific (19.48mA cm-2) and mass activity (76.74mAmg-1) at 1.59V versus RHE. Operando-EIS study evident that iCOP-CB[7]-2 commences OER at a relatively low applied potential of 1.5V versus RHE. These findings pave the way for a novel approach to synthesizing various mechanically interlocked molecules through straightforward solvothermal conditions.

ORR properties of PtM (M = Fe and Ni) ordered alloys with the effect of small molecules of cyanamide

Ordered Pt alloy electrocatalysts have a special geometric structure and exhibit excellent oxygen reduction reaction (ORR) catalytic performance. Herein, we successfully prepared PtFe/PtNi ordered alloy catalysts by thermal annealing method under the protection of the encapsulated shell formed by pyrolysis of cyanamide molecules as well as the effect of the N element entering into the alloy system to cause defects, and kept the average particle size below 4 nm. The ordered structure enhances the electronic interactions, keeps more Pt0 valence states present and improves the ORR catalytic activity. Under acidic conditions, the PtFe ordered alloy catalyst had a mass activity of 0.752 A mgPt−1 and a specific activity of 1.138 mA cmPt−2, both of which were superior to the commercial Pt/C and disordered PtFe alloy. Importantly, the strong interaction between ordered Pt and Fe prevents the leaching of Fe and maintains high mass activity after a long period of circulation. DFT calculations show that the ordered PtFe alloy has a low reaction energy barrier, which is favorable for ORR.

Constructing Zn-based MOF-MXene nanoarchitectures to stabilize ultrafine Pt nanocrystals with enhanced methanol oxidation performance

Although the development of direct methanol fuel cell technology is regarded as one rational option to against severe energy crises and environmental pollution, the low efficiency and considerable costs of current Pt-based anode catalysts largely impede the broad-scale commercialization. Herein, a convenient bottom-up approach is developed to the spatial construction of ultrafine Pt nanocrystals stabilized on a porous heterojunction matrix built from Zn-based metal organic frameworks and Ti3C2Tx MXene nanolamellas (Pt/ZIF-Ti3C2Tx) through the stepwise solvothermal reactions. The intercalation of metal organic frameworks produces plentiful cavities and channels for the dispersion and immobilization of small-sized Pt nanoparticles, while the incorporation of Ti3C2Tx nanosheets optimizes the Pt electronic structure and ensures a high electron conductivity. As a consequence, the as-acquired Pt/ZIF-Ti3C2Tx nanoarchitectures manifest exceptional electrocatalytic methanol oxidation abilities in terms of a large electrochemically active surface area of 110.5 m2 g−1, a high mass activity of 1900.1 mA mg−1, and preferable long-term stability, all of which are significantly superior to those of conventional Pt/carbon and Pt/unmodified Ti3C2Tx catalysts.

Ultralow-Loading Ruthenium-Iridium Fuel Cell Catalysts Dispersed on Zn-N Species-Doped Carbon.

Developing low-loading platinum-group-metal (PGM) catalysts is one of the key challenges in commercializing anion-exchange-membrane-fuel-cells (AEMFCs), especially for hydrogen oxidation reaction (HOR). Here, ruthenium-iridium nanoparticles being deposited on a Zn-N species-doped carbon carrier (Ru6Ir/Zn-N-C) are synthesized and used as an anodic catalyst for AEMFCs. Ru6Ir/Zn-N-C shows extremely high mass activity (5.87AmgPGM -1) and exchange current density (0.92mAcm-2), which is 15.1 and 3.9 times that of commercial Pt/C, respectively. Based on the Ru6Ir/Zn-N-C AEMFCs achieve a peak power density of 1.50Wcm-2, surpassing the state-of-the-art commercial PtRu catalysts and the power ratio of the normalized loading is 14.01WmgPGM anode -1 or 5.89W mgPGM -1 after decreasing the anode loading (87.49µgcm-2) or the total PGM loading (0.111mgcm-2), satisfying the US Department of Energy's PGM loading target. Moreover, the solvent and solute isotope separation method is used for the first time to reveal the kinetic process of HOR, which shows the reaction is influenced by the adsorption of H2O and OH-. The improvement of the hydrogen bond network connectivity of the electric double layer by adjusting the interfacial H2O structure together with the optimized HBE and OHBE is proposed to be responsible for the high HOR activity of Ru6Ir/Zn-N-C.

Antimony tin oxide supported iridium oxide nanocatalyst with bi-directional strains for oxygen evolution reaction in PEM electrolyzers

The use of proton exchange membrane (PEM) electrolyzers in H2 production encounters notable challenges related to the activity and stability of the oxygen evolution reaction (OER). To address these issues, we introduce antimony tin oxide as carriers to support a core–shell structured Sb0.3Ir0.7Ox@TB-IrOx, featuring twin boundaries (TB) with bi-directional (shear and axial) strains. This catalyst exhibits a remarkably low overpotential of 198 mV at 10 mA cm−2 for OER in 0.5 M H2SO4 and impressively maintains stability for 200 h. Moreover, Sb0.3Ir0.7Ox@TB-IrOx/Sb0.2Sn0.8O2 demonstrates an exceptionally high mass activity of 4.06 A mg Ir-1 (η = 270 mV). The improved catalytic activity and stability are attributed to the introduction of antimony, which brings the Ir 5d band center (εd) closer to the Fermi level and results in a smaller catalyst particle size, exposing more active sites. Furthermore, a PEM electrolyzer employing the Sb0.3Ir0.7Ox@TB-IrOx/Sb0.2Sn0.8O2 nanocatalyst maintains a cell voltage of 2 V at 2 A cm−2 and exhibits a stability more than 200 h.

Unveiling synergy of strain and ligand effects in metallic aerogel for electrocatalytic polyethylene terephthalate upcycling

Recently, there has been a notable surge in interest regarding reclaiming valuable chemicals from waste plastics. However, the energy-intensive conventional thermal catalysis does not align with the concept of sustainable development. Herein, we report a sustainable electrocatalytic approach allowing the selective synthesis of glycolic acid (GA) from waste polyethylene terephthalate (PET) over a Pd67Ag33 alloy catalyst under ambient conditions. Notably, Pd67Ag33 delivers a high mass activity of 9.7 A mgPd-1 for ethylene glycol oxidation reaction (EGOR) and GA Faradaic efficiency of 92.7 %, representing the most active catalyst for selective GA synthesis. In situ experiments and computational simulations uncover that ligand effect induced by Ag incorporation enhances the GA selectivity by facilitating carbonyl intermediates desorption, while the lattice mismatch-triggered tensile strain optimizes the adsorption of *OH species to boost reaction kinetics. This work unveils the synergistic of strain and ligand effect in alloy catalyst and provides guidance for the design of future catalysts for PET upcycling. We further investigate the versatility of Pd67Ag33 catalyst on CO2 reduction reaction (CO2RR) and assemble EGOR//CO2RR integrated electrolyzer, presenting a pioneering demonstration for reforming waste carbon resource (i.e., PET and CO2) into high-value chemicals.

PtPd Atomic Layer Shelled PdCu Hollow Nanoparticles on Partially Unzipped Carbon Nanotubes for Breaking the Activity-Stability Trade-Off toward the Hydrogen Oxidation Reaction in Alkaline Media.

Developing highly active yet stable catalysts for the hydrogen oxidation reaction (HOR) in alkaline media remains a significant challenge. Herein, we designed a novel catalyst of atomic PtPd-layer shelled ultrasmall PdCu hollow nanoparticles (HPdCu NPs) on partially unzipped carbon nanotubes (PtPd@HPdCu/W-CNTs), which can achieve a high mass activity, 5 times that of the benchmark Pt/C, and show exceptional stability with negligible decay after 20,000 cycles of accelerated degradation test. The atomically thin PtPd shell serves as the primary active site for the HOR and a protective layer that prevents Cu leaching. Additionally, the HPdCu substrate not only tunes the adsorption properties of the PtPd layer but also prevents corrosive Pt from reaching the interface between NPs and the carbon support, thereby mitigating carbon corrosion. This work introduces a new strategy that leverages the distinct advantages of multiple components to address the challenges associated with slow kinetics and poor durability toward the HOR.

Porous tungsten carbo-nitride supported Pt nanoparticles with high conductivity for efficient and stable hydrogen evolution reaction

Designing low-cost catalysts that offer both high mass activity and high cycling stability is crucial. Herein, a binder-free 3D self-supporting electrode composed of carbo-nitride tungsten supporting Pt nanoparticles (Pt@3DP-WNxC1-x/W) has been successfully synthesized for hydrogen evolution reaction in acid electrolyte. The tungsten carbo-nitride synthesized via a one-step heat treatment exhibits enhanced conductivity as a result of the carbonization process and optimizes the adsorption and desorption properties of WC towards H atoms through the incorporation of N atoms, thereby achieving an effective balance. Simultaneously, the N–Pt bond enhances electron transfer efficiency. This electrode exhibits outstanding electrochemical performance with a 219 mV overpotential at a current density of −300 mA cm−2. Its current density and mass activity is up to 75 mA cm−2 and 7.5 A·mgPt−1 at an overpotential of 100 mV, respectively, which are both 2.6 times higher than those of the 40% Pt/C electrode. In addition, it reveals a low Tafel slope of 38.3 mV dec−1 indicating rapid kinetics. Furthermore, the electrocatalyst shows only 3 mV day at −100 mA cm−2 after 10,000 cycles. Both theoretical calculation and experimental results show the promotion of catalytic efficiency of Pt@3DP-WNxC1-x/W brought by carbo-nitrition. This study offers a novel, efficient, and stable electrode design strategy.

Temperature-Induced Interface Hybridization of WC Boosts NiCu Activity for Alkaline Hydrogen Oxidation Reaction.

The development of non-precious hydrogen oxidation reaction (HOR) catalysts is a major challenge for the commercialization of Pt-free fuel cells. Herein, a temperature-induced phase hybridization method is reported that greatly improves the catalytic performance of NiCu alloy for the HOR. The migration of W atoms hybridizes the interface of tungsten oxide (WOx) and tungsten carbide (WC) at the onset reduction temperature of WOx, leading to a greatly weakened H binding energy and an optimized OH binding energy, which endows NiCuW/WOx-WC@WC with favorable stability and CO resistance during HOR. The hybridization catalysts deliver a high mass activity of 29.37 mA mg-1 Ni and reach a peak power of 298 mW.cm-2 in H2-O2 anion exchange membrane fuel cells (AEMFCs).

Ultrasmall Pd nanocrystals confined into Co-based metal organic framework-decorated MXene nanoarchitectures for efficient methanol electrooxidation

The natural scarcity and insufficient utilization of noble metal-based catalysts bring a heavy block in the way of the widespread applications of direct methanol fuel cells. Herein, we propose a feasible bottom-up approach to the construction of ultrasmall Pd nanocrystals confined into Co-based metal organic framework-decorated Ti3C2Tx MXene (Pd/MOF-MX) nanoarchitectures via a controllable solvothermal process. The ultrathin MXene nanolamellas and porous Co-based MOFs constitute an ideal hybrid carrier with high electron conductivity and large accessible surface areas, which not only facilitates the size restriction and uniform dispersion of Pd nanocrystals, but also ameliorates their intrinsic catalytic activity through the direct electronic interactions. By virtue of the pronounced synergistic coupling effects, the newly-developed Pd/MOF-MX nanoarchitectures exhibit markedly enhanced electrocatalytic properties towards the methanol oxidation reaction, including a large electrochemically active surface area of 116.7 m2 g−1, a high mass activity of 1700.4 mA mg−1 as well as a satisfactory long-term durability, which are superior to those of traditional Pd electrocatalysts anchored on carbon blacks, carbon nanotubes, graphene, and undecorated MXene matrixes.

Pt-Modified High Entropy Rare Earth Oxide for Efficient Hydrogen Evolution in pH-Universal Environments.

The development of efficient and stable catalysts for hydrogen production from electrolytic water in a wide pH range is of great significance in alleviating the energy crisis. Herein, Pt nanoparticles (NPs) anchored on the vacancy of high entropy rare earth oxides (HEREOs) were prepared for the first time for highly efficient hydrogen production by water electrolysis. The prepared Pt-(LaCeSmYErGdYb)O showed excellent electrochemical performances, which require only 12, 57, and 77 mV to achieve a current density of 100 mA cm-2 in 0.5 M H2SO4, 1.0 M KOH, and 1.0 M PBS environments, respectively. In addition, Pt-(LaCeSmYErGdYb)O has successfully worked at 400 mA cm-2 @ 60 °C for 100 h in 0.5 M H2SO4, presenting the high mass activity of 37.7 A mg-1Pt and turnover frequency (TOF) value of 38.2 s-1 @ 12 mV, which is far superior to the recently reported hydrogen evolution reaction (HER) catalysts. Density functional theory (DFT) calculations have revealed that the interactions between Pt and HEREO have optimized the electronic structures for electron transfer and the binding strength of intermediates. This further leads to optimized proton binding and water dissociation, supporting the highly efficient and robust HER performances in different environments. This work provides a new idea for the design of efficient RE-based electrocatalysts.