Mao Qian , Yakun Tang , Xiaohui Li , Yue Zhang , Weidong Jiang , Lang Liu
{"title":"Regulating the proximity of d-p band center in TiP2O7 by the crystalline-amorphous heterointerface to boost adsorption-catalysis for LiPSs in Li-S batteries","authors":"Mao Qian , Yakun Tang , Xiaohui Li , Yue Zhang , Weidong Jiang , Lang Liu","doi":"10.1016/j.jechem.2025.04.030","DOIUrl":"10.1016/j.jechem.2025.04.030","url":null,"abstract":"<div><div>The adsorption-catalysis ability of metal-based catalysts toward lithium polysulfides (LiPSs) is dominated by the position of their <em>d</em>-/<em>p</em>-band center. An available strategy to strengthen the <em>d</em>-<em>p</em> band center proximity of metal-based catalysts is to fabricate a crystalline-amorphous heterointerface, which markedly enhances LiPS conversion. The polyanionic pyrophosphate of TiP<sub>2</sub>O<sub>7</sub> serves as an efficient catalyst and ionic conductor for lithium-sulfur (Li-S) batteries. However, TiP<sub>2</sub>O<sub>7</sub> does not fully optimize sulfur redox reactivity due to limitations in factors such as the adsorption-catalysis of sulfur species, Li<sup>+</sup> diffusion, and electron transfer. Herein, we engineer the crystalline-amorphous heterointerface of TiP<sub>2</sub>O<sub>7</sub> combined with carbon nanotubes (CNTs) to facilitate electronic donation from C to TiP<sub>2</sub>O<sub>7</sub>. This interaction results in an upward shift of the Ti <em>d</em>, enhancing the proximity of the <em>d</em>-<em>p</em> band center in TiP<sub>2</sub>O<sub>7</sub>/CNTs. By utilizing TiP<sub>2</sub>O<sub>7</sub>/CNTs as both electrode and separator modifier, we optimize the LiPS conversion process, showing a comprehensive strategy to mitigate the diffusion of LiPSs and achieve the bidirectional redox reactions in Li-S batteries. Accordingly, the cell assembled by TiP<sub>2</sub>O<sub>7</sub>/CNTs delivers a satisfactory capacity of 835 mAh g<sup>−1</sup> after 300 cycles at 4 C and an impressive initial areal capacity of 3.52 mAh cm<sup>−2</sup> under the sulfur areal loading of 5 mg cm<sup>−2</sup> at 0.1 C. Additionally, the Li//Li cells utilizing TiP<sub>2</sub>O<sub>7</sub>/CNTs present a prolonged cycling life of up to 1800 h without voltage fluctuation and Li dendrite growth.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 458-467"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071136","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}
Zanbu Geng , Yang Yang , Yixi Wang , Wenqing Xu , Jun He , Tingyu Zhu
{"title":"Tailoring active hydroxyl group on FeZrOx nano-heterojunction for the enhanced low-temperature CO2-rich amine regeneration","authors":"Zanbu Geng , Yang Yang , Yixi Wang , Wenqing Xu , Jun He , Tingyu Zhu","doi":"10.1016/j.jechem.2025.04.019","DOIUrl":"10.1016/j.jechem.2025.04.019","url":null,"abstract":"<div><div>Catalytic regeneration is a key approach to solving high energy consumption issues in the amine-based CO<sub>2</sub> absorption method. Previous studies have shown that loaded acid sites (such as SO<sub>4</sub><sup>2−</sup>) are beneficial for promoting low-temperature CO<sub>2</sub>-rich amine regeneration, but their weak binding strength to the support results in limited catalyst life. Herein, we proposed an advanced catalyst modification strategy to maintain the active hydroxyl group (Zr–OH–Fe) via actively transferring electrons on the surface of FeZrO<em><sub>x</sub></em> nano-heterojunction. Combining in situ DRIFTS and DFT calculations, we revealed that the Zr–OH–Fe at the ZrO<sub>2</sub>-Fe<sub>2</sub>O<sub>3</sub> heterointerfaces exhibit enhanced proton-donating ability, with deprotonation energy reduced from 2.94 to 2.61 eV compared to Zr–OH (which should be called inert hydroxyl group). This improvement favors the rate-determining proton transfer step from RNH<sub>3</sub><sup>+</sup> to RNHCOO<sup>−</sup>. Surprisingly, it increased the CO<sub>2</sub> desorption rate by 10.5 times and reduced the energy consumption by 43.6% during amine regeneration. This work offers a practical strategy for improving the performance of low-temperature CO<sub>2</sub>-rich amine regeneration catalysts, and the low-cost recyclability of amine used in CO<sub>2</sub> capture.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 297-306"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143948436","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}
Peng Zhang , Shiyu Xu , Hao Li , Chenglin Cui , Shengyang Huang , Zhengyang Li , Hyun Jun Song , Lirui Mao , Chan-Hwa Chung , Ho Seok Park , Jin Yong Lee , Ji Man Kim , Pil J. Yoo
{"title":"Multi-metal synergistic integration for electronic structure regulation in schreibersite-type Mo2Fe0.8Ru0.2P electrocatalysts: exceptional enhancement of activity and stability for alkaline hydrogen evolution reaction","authors":"Peng Zhang , Shiyu Xu , Hao Li , Chenglin Cui , Shengyang Huang , Zhengyang Li , Hyun Jun Song , Lirui Mao , Chan-Hwa Chung , Ho Seok Park , Jin Yong Lee , Ji Man Kim , Pil J. Yoo","doi":"10.1016/j.jechem.2025.04.020","DOIUrl":"10.1016/j.jechem.2025.04.020","url":null,"abstract":"<div><div>Employing multiple metals for synergistic electronic structure regulation emerges as a promising approach to develop highly efficient and robust electrocatalysts for hydrogen evolution at ampere levels. In this study, a series of Schreibersite-type intermetallic compounds, particularly Mo<sub>2</sub>Fe<sub>0.8</sub>Ru<sub>0.2</sub>P, are synthesized through high-temperature solid-phase synthesis. Experimental results demonstrate that the integration of Ru significantly improves the kinetics of proton adsorption and desorption during the hydrogen evolution reaction (HER). Additionally, density functional theory (DFT) calculations and X-ray absorption near edge structure (XANES) analyses effectively corroborate the pronounced <em>d</em>-orbital hybridization of Fe within the structure, which facilitates the transfer of hydroxide ions and the maintenance of material durability during alkaline HER processes. Remarkably, Mo<sub>2</sub>Fe<sub>0.8</sub>Ru<sub>0.2</sub>P exhibits superior alkaline HER activity, characterized by an overpotential of merely 48 mV at a current density of 10 mA cm<sup>−2</sup>. After prolonged operation of 1000 h at high current densities (1.1 A cm<sup>−2</sup>), the activity decline remains minimal, under 4% (with overpotential increasing from 258 mV to 268 mV). These results demonstrate the potential of strategically combining metallic elements to design high-performance industrial-grade electrocatalysts.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 665-674"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105931","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":"A method to address the challenges of charging conditions on incremental capacity analysis: An ICA-compensation technique incorporating current interrupt methods","authors":"Jinghua Sun , Josef Kainz","doi":"10.1016/j.jechem.2025.03.092","DOIUrl":"10.1016/j.jechem.2025.03.092","url":null,"abstract":"<div><div>The incremental capacity analysis (ICA) technique is notably limited by its sensitivity to variations in charging conditions, which constrains its practical applicability in real-world scenarios. This paper introduces an ICA-compensation technique to address this limitation and propose a generalized framework for assessing the state of health (SOH) of batteries based on ICA that is applicable under differing charging conditions. This novel approach calculates the voltage profile under quasi-static conditions by subtracting the voltage increase attributable to the additional polarization effects at high currents from the measured voltage profile. This approach’s efficacy is contingent upon precisely acquiring the equivalent impedance. To obtain the equivalent impedance throughout the batteries’ lifespan while minimizing testing costs, this study employs a current interrupt technique in conjunction with a long short-term memory (LSTM) network to develop a predictive model for equivalent impedance. Following the derivation of ICA curves using voltage profiles under quasi-static conditions, the research explores two scenarios for SOH estimation: one utilizing only incremental capacity (IC) features and the other incorporating both IC features and IC sampling. A genetic algorithm-optimized backpropagation neural network (GA-BPNN) is employed for the SOH estimation. The proposed generalized framework is validated using independent training and test datasets. Variable test conditions are applied for the test set to rigorously evaluate the methodology under challenging conditions. These evaluation results demonstrate that the proposed framework achieves an estimation accuracy of 1.04% for RMSE and 0.90% for MAPE across a spectrum of charging rates ranging from 0.1 C to 1 C and starting SOCs between 0% and 70%, which constitutes a major advancement compared to established ICA methods. It also significantly enhances the applicability of conventional ICA techniques in varying charging conditions and negates the necessity for separate testing protocols for each charging scenario.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 65-80"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143895815","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":"The rise of perovskite solar cells-based integrated photovoltaic energy conversion-storage systems","authors":"Yajie Wang , Fei Zhang","doi":"10.1016/j.jechem.2025.04.021","DOIUrl":"10.1016/j.jechem.2025.04.021","url":null,"abstract":"<div><div>Perovskite solar cells (PSCs) are revolutionizing the renewable energy sector due to their exceptional efficiency under varying light intensity and potential for cost-effective large-scale manufacturing. With the rapid development of lithium-ion batteries (LIBs) and supercapacitors (SCs), integrating PSCs with these energy storage devices to provide a sustained energy supply is a promising approach, particularly in light of the intermittent nature of solar radiation and indoor lighting. This review first discusses the key parts of the PSCs-based integrated photovoltaic energy conversion-storage systems (IPECS), including PSCs, LIBs, SCs, and integration technologies. We also summarize the latest research progress in IPECS, focusing on the advancements of PSCs in combination with LIBs, SCs, and other devices. Ultimately, we propose a perspective on boosting opportunities and addressing the challenges for the future design of PSCs-based IPECS.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 317-331"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143948439","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":"β-Cyclodextrin inducing confinement effect enabling spherical Na3V2(PO4)3 with multielectron reaction and superior performance at extreme conditions for sodium-ion batteries","authors":"Shuming Zhang, Tao Zhou, Hongen Shi, Yanjun Chen","doi":"10.1016/j.jechem.2025.04.023","DOIUrl":"10.1016/j.jechem.2025.04.023","url":null,"abstract":"<div><div>Currently, simultaneous regulation of external morphology and internal electronic structure for Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub> (NVP) is rarely realized. Herein, complexes of β-cyclodextrin (βCD) and ethylenediaminetetraacetic acid ferric sodium salt (EDTAFeNa) are utilized for the one-step preparation of NVP with spherical morphology as well as Fe substitution. βCD is initially hydrolyzed into glucose, and then carbon microspheres with numerous pores are formed through continuous dehydration and carbonization. The intermediate hydroxymethylfurfural is rich in active functional groups, which are attractive for the V/P-contained raw materials. Accordingly, the nucleation sites for NVP are successfully limited in the spherical framework, possessing a superior surface area of 97.15 g m<sup>−2</sup>. Furthermore, the beneficial Fe in EDTAFeNa enters into the NVP bulk to construct a novel Fe-doped Na<sub>3</sub>V<sub>1.95</sub>Fe<sub>0.05</sub>(PO<sub>4</sub>)<sub>3</sub> (NVP/β-ISC) material. Fe-substitution induces significant optimizations of electronic structure for NVP, which has been verified by the newly generated abundant oxygen vacancies and extended V–O bond length. Moreover, a multielectron reaction is activated, resulting from the V<sup>4+</sup>/V<sup>5+</sup> redox couple. The charge compensation mechanism of NVP/β-ISC is also deeply investigated. Density functional theory (DFT) calculations theoretically elaborate the mechanism of Fe-doping. Consequently, NVP/β-ISC reveals superior sodium storage performance in both half and full cells and even at different extreme conditions (needling, soaking, bending, and freezing).</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 138-153"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143906082","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}
Shuaikang Dai , Zuosu Qin , Yuanhang Gao , Tao Zhang , Renfei Zhao , Yuelin Li , Gen Chen , Xiaozhong Zhou
{"title":"Dual-protection of cathode from HF corrossion enabling high-performance lithium metal batteries","authors":"Shuaikang Dai , Zuosu Qin , Yuanhang Gao , Tao Zhang , Renfei Zhao , Yuelin Li , Gen Chen , Xiaozhong Zhou","doi":"10.1016/j.jechem.2025.04.028","DOIUrl":"10.1016/j.jechem.2025.04.028","url":null,"abstract":"<div><div>Lithium metal batteries (LMBs) encounter substantial challenges related to hydrogen fluoride (HF)-induced degradation of electrode materials and interfacial instability. The predominant sources of HF are attributed to the hydrolysis of lithium hexafluorophosphate (LiPF<sub>6</sub>) in the electrolyte and the decomposition of fluorine-containing solvents, which result in transition metal dissolution, rapid capacity fading, and overall battery performance deterioration. To mitigate these issues, we introduce a dual-protection strategy via the synergistic incorporation of pentafluorophenyl trifluoroacetate (PFTFA) and lithium difluoro(oxalato)borate (LiDFOB) additives, achieving both chemical HF capture and physical HF defense. The optimized electrolyte system not only promotes the formation of a robust cathode-electrolyte interphase layer enriched with LiF and LiB<em><sub>x</sub></em>O<em><sub>y</sub></em> compounds but also effectively scavenges HF through PFTFA coordination, thereby ensuring enhanced cathode stability. Consequently, the Li||LiNi<sub>0.8</sub>Co<sub>0.1</sub>Mn<sub>0.1</sub>O<sub>2</sub> (NCM811) cells demonstrate remarkable cyclic stability with 80% capacity retention over 420 cycles at the cutoff voltage of 4.4 V under 1 C rate, whereas conventional carbonate-based electrolytes only retain 54.8% capacity after 150 cycles under identical conditions. Even under high voltage conditions (4.8 V, 0.5 C), the developed electrolyte maintains 77.8% capacity retention over 200 cycles. This work provides valuable insights into the rational design of multifunctional electrolyte additives for high-performance LMBs.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 173-180"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143906085","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}
Jinzhen Huang , Erica D. Clinton , Kenneth Crossley , Juliana Bruneli Falqueto , Thomas J. Schmidt , Emiliana Fabbri
{"title":"Uncovering the catalyst/electrolyte interfacial process by frequency dispersion of capacitance","authors":"Jinzhen Huang , Erica D. Clinton , Kenneth Crossley , Juliana Bruneli Falqueto , Thomas J. Schmidt , Emiliana Fabbri","doi":"10.1016/j.jechem.2025.04.024","DOIUrl":"10.1016/j.jechem.2025.04.024","url":null,"abstract":"<div><div>Electrochemical impedance spectroscopy (EIS) is a widely used technique to monitor the electrical properties of a catalyst under electrocatalytic conditions. Although it is extensively used for research in electrocatalysis, its effectiveness and power have not been fully harnessed to elucidate complex interfacial processes. Herein, we use the frequency dispersion parameter, <em>n</em>, which is extracted from EIS measurements (<em>C</em><sub>s</sub> = <em>af<sup>n</sup></em><sup>+1</sup>, −2 < <em>n</em> < −1), to describe the dispersion characteristics of capacitance and interfacial properties of Co<sub>3</sub>O<sub>4</sub> before the onset of oxygen evolution reaction (OER) in alkaline conditions. We first prove that the <em>n</em>-value is sensitive to the interfacial electronic changes associated with Co redox processes and surface reconstruction. The <em>n</em>-value decreases by increasing the specific/active surface area of the catalysts. We further modify the interfacial properties by changing different components, i.e., replacing the proton with deuterium, adding ethanol as a new oxidant, and changing the cation in the electrolyte. Intriguingly, the <em>n</em>-value can identify different influences on the interfacial process of proton transfer, the decrease and blocking of oxidized Co species, and the interfacial water structure. We demonstrate that the <em>n</em>-value extracted from EIS measurements is sensitive to the kinetic isotope effect, electrolyte cation, adsorbate surface coverage of oxidized Co species, and the interfacial water structure. Thus, it can be helpful to differentiate the multiple factors affecting the catalyst interface. These findings convey that the frequency dispersion of capacitance is a convenient and useful method to uncover the interfacial properties under electrocatalytic conditions, which helps to advance the understanding of the interface-activity relationship.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 199-209"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143905999","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}
Mingwei Zhu , Danlin Ruan , Xin Zhao , Jiawei Song , Jiahao Cheng , Wenjian Shen , Wangnan Li , Guijie Liang , Ying Liang , Yong Peng , Bin Li , Yi-Bing Cheng
{"title":"Triphenylphosphine oxide additive regulates the growth of perovskite films by evaporation-spraying technique for high-efficiency large-area solar cell modules","authors":"Mingwei Zhu , Danlin Ruan , Xin Zhao , Jiawei Song , Jiahao Cheng , Wenjian Shen , Wangnan Li , Guijie Liang , Ying Liang , Yong Peng , Bin Li , Yi-Bing Cheng","doi":"10.1016/j.jechem.2025.04.022","DOIUrl":"10.1016/j.jechem.2025.04.022","url":null,"abstract":"<div><div>Premature perovskite films rapidly form at the FAI/PbI<sub>2</sub> interface, inhibiting further reactions between FAI and PbI<sub>2</sub> during the fabrication of perovskite films via the evaporating-spraying hybrid method according to our previous research. In this research, triphenylphosphine oxide (TPPO) was proved to be an effective coordinator that reduces the reaction rate between FAI and PbI<sub>2</sub> at the initial stage, which can be attributed to the hydrogen (H) bonds between FA<sup>+</sup> and TPPO, and coordinate bonds between TPPO and PbI<sub>2</sub>. Additionally, the quality of perovskite films improved significantly: the trap state density decreased from 1.6 × 10<sup>18</sup> to 3.17 × 10<sup>17</sup> cm<sup>−3</sup>, while the crystal size increased from 740 to 940 nm. The champion perovskite device achieved a remarkable efficiency of 20.93% (0.09 cm<sup>2</sup>) and 16.75% (63.7 cm<sup>2</sup>), marking one of the highest reported results for the evaporating-spraying hybrid method. Moreover, the perovskite solar cells retained over 80% of their initial performances after 600 h of storage at 60 °C in a nitrogen environment without encapsulation. It also maintained approximately 90% of its initial performance after continuous illumination at 25 °C for 1400 h under the same conditions.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"108 ","pages":"Pages 468-476"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144071137","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}
Jinli Liu , Mo Zhang , Ling Tang , Simin Zhang , Jiayong Lu , Xu Yang , Yangming Lin
{"title":"Surface hybrid engineering of nanodiamonds for boosting electrocatalytic hydrogen peroxide production with high efficiency and stability","authors":"Jinli Liu , Mo Zhang , Ling Tang , Simin Zhang , Jiayong Lu , Xu Yang , Yangming Lin","doi":"10.1016/j.jechem.2025.04.026","DOIUrl":"10.1016/j.jechem.2025.04.026","url":null,"abstract":"<div><div>Hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) is an important chemical that can be sustainably produced through a two-electron pathway in the electrocatalytic oxygen reduction reaction (ORR). However, the high cost and low reaction efficiency of catalysts currently limit the widespread application of this technology. Developing high-selectivity and scalable catalysts and accurately identifying the reaction active sites remain challenges. In this work, we have developed a promising nanodiamond (ND) catalyst to achieve high-selectivity H<sub>2</sub>O<sub>2</sub> production by oxygen reduction. Through surface carbon hybridization regulation to identify specific oxygen-containing functional groups combined with titration, model<!--> <!-->catalysis and DFT methods, it is found that the presence of carbonyl groups inducing the surrounding carbon atoms exhibit an optimal *OOH adsorption strength, thus promoting the two-electron pathway in ORR. Specifically, dynamic evolution processes of carbonyl groups and key adsorbed intermediate products including O<sub>2</sub> (ads), superoxide anion *O<sub>2</sub><sup>−</sup>, and *OOH are monitored in situ spectroscopy. In the flow-cell device, ND catalyst realizes the high H<sub>2</sub>O<sub>2</sub> Faradaic efficiency around 92% with a rate activity up to 105 mol g<sub>C=O</sub><sup>−1</sup> h<sup>−1</sup>, surpassing among reported non-metallic catalysts. The total H<sub>2</sub>O<sub>2</sub> yield reaches to 23.79 mM after a ten-hour test, which is 2.56 times higher than that of carbonyl-passivated ND, demonstrating its potential in scale-up application. Both titration and model catalytic processes proposed in this study further offer methods of designing efficient electrocatalysts for H<sub>2</sub>O<sub>2</sub> production.</div></div>","PeriodicalId":15728,"journal":{"name":"Journal of Energy Chemistry","volume":"109 ","pages":"Pages 15-23"},"PeriodicalIF":13.1,"publicationDate":"2025-04-22","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144105840","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}