Journal of Energy Chemistry最新文献

{"title":"Construction of efficient electrodes for CO2RR through microenvironment regulation of hydrophobic ionomer","authors":"Qingfeng Chang ,&nbsp;Gong Zhang ,&nbsp;Jinxing Chen ,&nbsp;Xiaowei Du ,&nbsp;Chujun Wang ,&nbsp;Yuan Cai ,&nbsp;Yuzhe Du ,&nbsp;Peng Zhang ,&nbsp;Tuo Wang ,&nbsp;Jinlong Gong","doi":"10.1016/j.jechem.2025.04.040","DOIUrl":"10.1016/j.jechem.2025.04.040","url":null,"abstract":"<div><div>CO₂ reduction reaction (CO₂RR) electrolyzers based on gas diffusion electrode (GDE) enable the direct mass transfer of CO₂ to the catalyst surface for participation in the reaction, thereby establishing an efficient three-phase reaction interface that significantly enhances current density. However, current hydrophobic modification methods face difficulties in achieving precise and substantial control over wettability, and the hydrophobic modifiers tend to significantly impair the conductivity of the electrode and ion transport capabilities. This study employs Nafion ionomers to hydrophobically modify the three-dimensional catalyst layer, revealing the bifunctionality of Nafion. The fluorinated backbone of Nafion ensures the hydrophobicity of the entire catalyst layer, while its sulfonic acid groups promote ion transport, without significantly affecting the conductivity of the electrode. Furthermore, by employing modifiers with distinct wettability characteristics, a highly efficient and large-scale manipulation of the hydrophilic/hydrophobic properties of the catalyst layer was successfully realized. The electrode, constructed with silver nanopowder as a representative catalyst and modified with the hydrophobic ionomer Nafion, exhibits a substantial enhancement in both catalytic activity and durability. The optimized electrode exhibited exceptional electrocatalytic performance in both flow cell and membrane electrode assembly (MEA) configurations. Notably, in the MEA, the electrode achieved a remarkable CO Faradaic efficiency (FE) of 93.3% at a total current density of 200 mA cm⁻², while maintaining stable operation for over 62 h.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 373-380"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Sintering- and water-resistant perovskite quantum dots supported by inorganic materials for enhanced luminescence","authors":"Meng Wu ,&nbsp;Lingxiang Sun ,&nbsp;Yanjie Zhang ,&nbsp;Feng Hong ,&nbsp;Xunzhu Jiang ,&nbsp;Xiuping Wu ,&nbsp;Chunwen Ye ,&nbsp;Jingjie Yu ,&nbsp;Bing Li ,&nbsp;Botao Qiao","doi":"10.1016/j.jechem.2025.04.041","DOIUrl":"10.1016/j.jechem.2025.04.041","url":null,"abstract":"<div><div>Metal halide perovskite quantum dots (MHPQDs) have attracted intensive interest because of their unique optoelectronic properties. Their undesirable degradation upon exposure to humidity and/or heat, however, poses a dear challenge for the practical applications. Herein we report a facile strategy to develop sintering-resistant MHPQDs, e.g. CsPbBr₃, by localizing them on the surface of inorganic support such as hydroxyapatite (HAP). The chemical interaction between CsPbBr₃ quantum dots (QDs) and HAP support originates from the occupation of Br vacancies in CsPbBr₃ by the –O⁻ on the surface of HAP support, which not only stabilizes the small particle sizes (∼2.2 nm) of CsPbBr₃ QDs upon high-temperature (up to 400 °C) calcination but also greatly enhances its photoluminescence emission intensity by about 150 times. Interestingly, the supported CsPbBr₃ QDs decorated by cetyltrimethylammonium bromide can further produce water-resistant CsPbBr₃@CsPb₂Br₅ QDs. The obtained sintering-resistant hydroxyapatite-supported CsPbBr₃@CsPb₂Br₅ QDs can be used to fabricate green light emitting diodes (LED) devices with high luminous intensity for medicolegal identification, flexible luminescence film for display, and potential fluorescent label for bioimaging/biosensing applications. This work demonstrates a novel strategy to design and develop robust all-inorganic QDs composites that may find wide applications in diverse environmental conditions, including high temperature and/or high humidity.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 508-516"},"PeriodicalIF":13.1,"publicationDate":"2025-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072589","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Three-dimensional covalent organic framework photocatalyst with asymmetrically coordinated single-atom cobalt for highly efficient CO2 reduction reactions","authors":"Wuqing Luo ,&nbsp;Jia Chen ,&nbsp;Zhuozhuo Tang ,&nbsp;Baopeng Yang ,&nbsp;Guoxin Chen ,&nbsp;Shengyao Wang ,&nbsp;Gen Chen ,&nbsp;Min Liu ,&nbsp;Hong Xu ,&nbsp;Jinhua Ye ,&nbsp;Ning Zhang","doi":"10.1016/j.jechem.2025.04.032","DOIUrl":"10.1016/j.jechem.2025.04.032","url":null,"abstract":"<div><div>Three-dimensional (3D) covalent organic frameworks (COFs) have attracted extensive attention as photocatalysts for CO₂ reduction reactions. Introducing metal atoms is essential for enhancing activity, but previous metal sites in 3D COFs predominantly exhibit symmetrical coordination, making them unsuitable for CO₂ activation. Here, we design a 3D COF with 2,2′-pyridine linked around tetra-(4-anilyl)methane (TCM-Bpy-COF), where Co²⁺ is asymmetrically coordinated by bipyridine and acetates (TCM-Bpy-COF-CoAc). The TCM-Bpy-COF-CoAc exhibits outstanding photocatalytic CO₂ reduction performance under weak visible light, achieving a CO evolution rate of 26,650 μmol g⁻¹ h⁻¹ under 5 W of light-emitting-diode (LED) lamp and high apparent quantum efficiency. The performance far exceeds that of symmetrically coordinated bipyridine-Co-bipyridine TCM-Bpy-COF and surpasses most reported COF-based photocatalysts. In-situ spectral characterizations and theoretical calculations show that asymmetric N, O-coordination around the Co²⁺ center polarizes electron density and lowers reaction energy barriers of *COOH intermediates, enhancing the conversion of CO₂ to CO. This work inspires the design of 3D COF-based photocatalysts with highly catalytic efficiency.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 400-409"},"PeriodicalIF":13.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071204","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Switching the product selectivity from methane to methanol in CO2 hydrogenation via Cu-modified vacancy engineering at MoS2 edge sites","authors":"Guanghui Zhang ,&nbsp;Xin Meng ,&nbsp;Hao Wang ,&nbsp;Zhiqun Wang ,&nbsp;Hui Gao ,&nbsp;Mingrui Wang ,&nbsp;Chunshan Song ,&nbsp;Xinwen Guo","doi":"10.1016/j.jechem.2025.04.038","DOIUrl":"10.1016/j.jechem.2025.04.038","url":null,"abstract":"<div><div>The catalytic hydrogenation of carbon dioxide (CO₂) to methanol (CH₃OH) represents a promising strategy for mitigating carbon emissions and closing the carbon cycle. This study demonstrates that the incorporation of Cu into MoS₂ catalysts significantly enhances methanol selectivity and productivity. Through a combination of transmission electron microscope, X-ray diffraction, Raman, electron paramagnetic resonance, X-ray photoelectron spectroscopy, diffuse reflectance Infrared Fourier transform spectroscopy, X-ray absorption spectroscopy, temperature-programmed desorption, and kinetic analysis, we reveal that Cu modifies edge sulfur vacancies, thereby suppressing methane formation and promoting methanol synthesis. At 220 °C and 5 MPa, the 2%Cu/MoS₂ catalyst achieves 85.5% selectivity toward CH₃OH, and the methanol formation rate reaches 7.88 mmol g⁻¹_cat h⁻¹ (0.256 mmol <span><math><mrow><msubsup><mrow><mi>m</mi></mrow><mrow><msub><mrow></mrow><mrow><msub><mrow><mi>MoS</mi></mrow><mrow><mn>2</mn></mrow></msub></mrow></msub></mrow><mrow><mo>-</mo><mn>2</mn></mrow></msubsup></mrow></math></span> h⁻¹), representing the highest performance among MoS₂-based catalysts under comparable conditions. This work provides an efficient and potentially scalable approach for designing advanced MoS₂-based catalysts for CO₂ hydrogenation.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 286-296"},"PeriodicalIF":13.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143943292","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"f-p-d coupling-induced bonding covalency boosts CC coupling in electrocatalytic CO2 reduction over ErOCu sites","authors":"Maoyin Wang ,&nbsp;Yuhang Huang ,&nbsp;Lu Song ,&nbsp;Ruilin Wei ,&nbsp;Shuya Hao ,&nbsp;Zhengzheng Liu ,&nbsp;Cejun Hu ,&nbsp;Bin Li ,&nbsp;Ximeng Lv ,&nbsp;Pei Yuan ,&nbsp;Gengfeng Zheng","doi":"10.1016/j.jechem.2025.03.039","DOIUrl":"10.1016/j.jechem.2025.03.039","url":null,"abstract":"<div><div>The copper-based electrocatalysts feature attractive potentials of converting CO₂ into multi-carbon (C₂₊) products, while the instability of Cu<img>O often induces the reduction of Cu⁺/Cu⁰ catalytic sites at the cathode and refrains the capability of stable electrolysis especially at high powers. In this work, we developed an Erbium (Er) oxide-modified Cu (Er<img>O<img>Cu) catalyst with enhanced covalency of Cu<img>O and more stable active sites. The <em>f</em>-<em>p</em>-<em>d</em> coupling strengthens the covalency of Cu<img>O, and the stability of Cu⁺ sites under electroreduction condition is critical for promoting the C<img>C coupling and improving the C₂₊ product selectivity. As a result, the Er<img>O<img>Cu sites exhibited a high Faradaic efficiency of C₂₊ products (FE_C2+) of 86 % at 2200 mA cm⁻², and a peak partial current density of |<em>j</em>_C2+| of 1900 mA cm⁻², comparable to the best reported values for the CO₂-to-C₂₊ electroreduction. The CO₂ electrolysis by the Er<img>O<img>Cu sites was further scaled up to 100 cm² to achieve high-power (∼200 W) electrolysis with ethylene production rate of 16 mL min⁻¹.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 239-245"},"PeriodicalIF":13.1,"publicationDate":"2025-04-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143923479","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"High-density oxygen-deficient CuO induced from structural reconstruction for efficient furfural oxidation coupled with hydrogen evolution","authors":"Hanshuai Xu ,&nbsp;Yun Han ,&nbsp;Qilong Wu ,&nbsp;Hao Chen ,&nbsp;Xinyi Shen ,&nbsp;Mingming Zhan ,&nbsp;Qingzhu Shu ,&nbsp;Xin Wang ,&nbsp;Huajun Zheng ,&nbsp;Lingxia Zheng ,&nbsp;Yi Jia","doi":"10.1016/j.jechem.2025.04.037","DOIUrl":"10.1016/j.jechem.2025.04.037","url":null,"abstract":"<div><div>The electrocatalytic furfural oxidation reaction (FFOR) represents an economical and promising technology to replace conventional oxygen evolution reaction, enabling the co-production of high value chemicals and H₂. Regulating the adsorption of furfural (FF) and OH⁻ species holds paramount importance in enhancing the overall performance. Herein, we have developed a unique CuO catalyst enriched with oxygen vacancies (O_v-CuO) resulting from the electrochemical reconstruction of <em>α</em>-Cu₂S, which demonstrates exceptional FFOR performance, with a conversion of 95.3%, near-perfect selectivity and Faraday efficiency (FE) for furoic acid (FA) at 1.475 V vs. RHE. The study provides detailed comparison of the structural evolution of different sulfide precatalysts and their impact on FFOR. Furthermore, it delves into the structure-activity relationship through a combination of characterization and theoretical calculations. The O_v-CuO not only enhances OH⁻ adsorption, changes the rate-determining step, but also reduces the reaction energy barrier toward FFOR. Additionally, a much lower cell voltage is required to coproduce FA and hydrogen in the two-electrode co-electrolysis system. This work would provide valuable insights into the reaction mechanism of FFOR on Cu based catalysts and establish guidelines for designing defective electrocatalysts for biomass conversion.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 584-592"},"PeriodicalIF":13.1,"publicationDate":"2025-04-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144089205","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Photothermal-driven enhancing photocatalysis and photoelectrocatalysis: advances and perspectives","authors":"Wenfeng Li,&nbsp;Guocheng Lv,&nbsp;Meng Liu,&nbsp;Fanyue Zhao,&nbsp;Pengfei Shuai,&nbsp;Yanmei Feng,&nbsp;Daimei Chen,&nbsp;Libing Liao","doi":"10.1016/j.jechem.2025.04.027","DOIUrl":"10.1016/j.jechem.2025.04.027","url":null,"abstract":"<div><div>Photocatalysis (PC) and photoelectrocatalysis (PEC) represent promising and efficient avenues for harnessing solar energy to produce sustainable clean energy products and environmental remediation. Yet the current reaction efficiencies remain inadequate, limiting their efficiencies for practice. Despite the growing interest in photothermal-driven PC/PEC systems, there is no comprehensive review that systematically summarises the role of the photothermal effect in bridging the gap between PC and PEC efficiencies. This review initially introduces the fundamental principles of PC and PEC, alongside the primary photothermal materials and relevant conversion mechanisms. Subsequently, the key influences of photothermal effects on PC and PEC performance (e.g., light absorption, charge separation and transport, and surface reactions) and optimization strategies are discussed. In addition, the latest advancements in solar photothermal conversion are discussed, mainly focused on the widely application of different types of photothermal drive PC and PEC applications, such as PC and PEC oxygen evolution reaction (OER), hydrogen evolution reaction (HER), CO₂ reduction reaction (CO₂ RR), pollutant degradation, and sterilization, serving to illustrate the widespread applicability of the photothermal conversion. Finally, the development prospects and challenges of photothermal-assisted PC and PEC are discussed from the perspective of basic research and practical application. This work provides a timely and systematic framework to guide the rational design of photothermal-enhanced PC/PEC systems for sustainable energy and environmental applications.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 332-360"},"PeriodicalIF":13.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144068006","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electronegativity-induced modulation of polysulfide adsorption in halogen-doped Ni2P to accelerate conversion kinetics for lithium-sulfur batteries","authors":"Lin Peng ,&nbsp;Yu Bai ,&nbsp;Hang Li ,&nbsp;Zhenhua Wang ,&nbsp;Kening Sun","doi":"10.1016/j.jechem.2025.04.034","DOIUrl":"10.1016/j.jechem.2025.04.034","url":null,"abstract":"<div><div>Heteroatom doping has emerged as a powerful strategy to optimize the catalytic and adsorption abilities of electrocatalysts by regulating the electronic structure, thereby enabling the development of efficient electrocatalysts for lithium-sulfur (Li-S) batteries. However, the correlation between the properties of doped atoms and adsorption-catalytic ability, as well as the interconnection between adsorption strength and catalytic activity, remains underexplored. Herein, we employed halogen atoms (F, Cl, and Br) with different electronegativities to dope nickel phosphide (Ni₂P), aiming to modulate the adsorption properties toward lithium polysulfides (LiPSs). We systematically explored the relationship between the electronegativity of the doping atoms and the adsorption strength, followed by exploring the connection between adsorption and catalytic capabilities. Combined experimental and theoretical analyses reveal that doping halogen atoms effectively strengthens <em>d</em>-<em>p</em> orbital hybridization between Ni atoms and S atoms, thereby enhancing LiPSs anchoring and conversion. Specifically, the chemical adsorption capability is enhanced as the electronegativity of the doped atoms increases. Moreover, the catalytic activity presents a volcano-like trend with the enhancement of adsorption performance, wherein the activity initially increases and subsequently diminishes. Therefore, Cl-doped Ni₂P with moderate chemisorption ability exhibits optimal redox kinetics in bidirectional sulfur conversion. Consequently, the Li-S batteries with Cl-Ni₂P-separators deliver a high-rate capacity of 790 mAh g⁻¹ at 5 C and achieve a remarkable areal capacity of 7.36 mAh cm⁻² under practical conditions (sulfur loading: 7.10 mg cm⁻²; electrolyte/sulfur (E/S) ratio: 5 μL mg⁻¹). This work uncovers the significance of achieving a balance between adsorption and catalytic capabilities, offering insights into designing efficient electrocatalysts for lithium-sulfur batteries.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 190-198"},"PeriodicalIF":13.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143912863","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electro-chemo-mechanics interplays caused by solid electrolyte-lithium anode interface roughness in all-solid-state batteries","authors":"Chunhao Yuan ,&nbsp;Jing Wu ,&nbsp;Wenjing Zhang ,&nbsp;Menghui Han ,&nbsp;Yikai Jia","doi":"10.1016/j.jechem.2025.04.033","DOIUrl":"10.1016/j.jechem.2025.04.033","url":null,"abstract":"<div><div>Solid-to-solid interfacial issues are one of the most intractable problems hindering the practical application of all-solid-state batteries (ASSBs). The interfacial instability behaviors caused by the rough interface between lithium anode and solid electrolyte (SE) involve complicated electro-chemo-mechanics interplays and their quantitative relationships still remain unclear. The three-dimensional electro-chemo-mechanical coupled model with randomly generated rough lithium-SE interface is developed in this study to investigate the effects of interface roughness on the interfacial failure behaviors. Results demonstrate that the existence of a rough lithium-SE interface causes the highly concentrated strain, GPa-level stress, and localized current density at the protruding tips, probably inducing dendrite formation and interface cracking. The interface roughness effect is much more pronounced in lithium anode than graphite anode due to their different Li storage mechanisms, i.e., surface deposition and Li intercalation. Excessive stack pressure (&gt;50 MPa) magnifies the stress effect on overpotential to enlarge the current density localization and deteriorate the interfacial instability issues. Reducing interface roughness through surface treatment, together with regulation of external operation conditions, can effectively improve interfacial stability performance. The results provide an in-depth understanding of the underlying electro-chemo-mechanical coupling mechanism caused by the rough anode-SE interface and bring more insights into further improvement of ASSBs’ enhanced reliability and longevity.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 495-507"},"PeriodicalIF":13.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144072592","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Electronic modulation of MOF-engineered bimetallic phosphides for cost-effective ampere-level water splitting and continuous hydrogen production via supercapacitor integration","authors":"Mohd Afshan,&nbsp;Naveen Kumar,&nbsp;Subhabrata Das,&nbsp;Harini E.M,&nbsp;Daya Rani,&nbsp;Soumyadip Sharangi,&nbsp;Mansi Pahuja,&nbsp;Shumile Ahmed Siddiqui,&nbsp;Seema Rani,&nbsp;Nikita Chaudhary,&nbsp;Chandan Bera,&nbsp;Kaushik Ghosh","doi":"10.1016/j.jechem.2025.04.018","DOIUrl":"10.1016/j.jechem.2025.04.018","url":null,"abstract":"<div><div>Engineering a phosphide-based multifunctional heterostructure with high redox activity, stability, and efficient charge kinetics for both supercapacitors and water splitting remains challenging due to sluggish reaction kinetics and structural instability. This study overcomes these challenges by implementing a rapid, energy-efficient approach to develop a MOF-modulated MnP@Cu₃P heterostructure via a hydrothermal process followed by high-temperature phosphorization. The heterostructure demonstrates superior redox activity with enhanced stability and improved charge kinetics achieving a high specific capacity of 1131 C g⁻¹ as supported by density functional theory findings of increased DOS near the Fermi level. The flexible supercapacitor achieves a peak energy density of 99.20 Wh kg⁻¹ and power density of 15.40 kW kg⁻¹. Simultaneously, it shows exceptional hydrogen evolution reaction performance with an overpotential of <em>η</em>₁₀ = 44 mV and <em>η</em>₁₀₀₀ = 225 mV, attributed to electron transfer from Cu to Mn via P bridging, which shifts the active centers from Mn and Cu sites to the P site, confirmed by lowest Δ<em>G</em>_H* value of −0.16 eV. The overall water-splitting in full-cell electrocatalyzer delivers cell voltage of <em>E</em>₂₀ = 1.48 V and <em>E</em>₁₀₀₀ = 1.88 V and setting a new standard in solar-to-hydrogen efficiency of 20.02%. The electrolyzer cell maintained prolonged stability at industrial-scale current densities of 1.0 A cm⁻² under alkaline electrolysis achieving an estimated hydrogen production cost of INR 146.7 or US$ 1.67 per kilogram aligning with the cost target of $ 2/kg by 2026 established by the Clean Hydrogen Electrolysis Program, U.S. department of energy. Furthermore, real-phase demonstration highlights the uninterrupted hydrogen production till 6-minutes via connecting this electrocatalyzer with photovoltaic-charged supercapacitors effectively addressing solar intermittency and gas fluctuations challenges in water-electrolysis.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 221-238"},"PeriodicalIF":13.1,"publicationDate":"2025-04-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143923481","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}