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| 1 | Recent Advances in Single-Atom Electrocatalysts for Oxygen Reduction Reaction显示文摘Oxygen reduction reaction(ORR)plays significant roles in electrochemical energy storage and conversion systems as well as clean synthesis of fine chemicals.However,the ORR process shows sluggish kinetics and requires platinum-group noble metal catalysts to accelerate the reaction.The high cost,rare reservation,and unsatisfied durability significantly impede large-scale commercialization of platinum-based catalysts.Single-atom electrocatalysts(SAECs)featuring with well-defined structure,high intrinsic activity,and maximum atom efficiency have emerged as a novel field in electrocatalytic science since it is promising to substitute expensive platinum-group noble metal catalysts.However,finely fabricating SAECs with uniform and highly dense active sites,fully maximizing the utilization efficiency of active sites,and maintaining the atomically isolated sites as single-atom centers under harsh electrocatalytic conditions remain urgent challenges.In this review,we summarized recent advances of SAECs in synthesis,characterization,oxygen reduction reaction(ORR)performance,and applications in ORR-related H_(2)O_(2)production,metal-air batteries,and low-temperature fuel cells.Relevant progress on tailoring the coordination structure of isolated metal centers by doping other metals or ligands,enriching the concentration of single-atom sites by increasing metal loadings,and engineering the porosity and electronic structure of the support by optimizing the mass and electron transport are also reviewed.Moreover,general strategies to synthesize SAECs with high metal loadings on practical scale are highlighted,the deep learning algorithm for rational design of SAECs is introduced,and theoretical understanding of active-site structures of SAECs is discussed as well.Perspectives on future directions and remaining challenges of SAECs are presented. | Junxing Han Juanjuan Bian Chunwen Sun | 2020 | Research2020，，1： | 6 |
| 2 | Benzoate anions-intercalated NiFe-layered double hydroxide nanosheet array with enhanced stability for electrochemical seawater oxidation显示文摘Seawater electrolysis is an extremely attractive approach for harvesting clean hydrogen energy,but detrimental chlorine species(i.e.,chloride and hypochlorite)cause severe corrosion at the anode.Here,we report our recent finding that benzoate anions-intercalated NiFe-layered double hydroxide nanosheet on carbon cloth(BZ-NiFe-LDH/CC)behaves as a highly efficient and durable monolithic catalyst for alkaline seawater oxidation,affords enlarged interlayer spacing of LDH,inhibits chlorine(electro)chemistry,and alleviates local pH drop of the electrode.It only needs an overpotential of 320 mV to reach a current density of 500 mA·cm^(−2)in 1 M KOH.In contrast to the fast activity decay of NiFe-LDH/CC counterpart during long-term electrolysis,BZ-NiFe-LDH/CC achieves stable 100-h electrolysis at an industrial-level current density of 500 mA·cm^(−2)in alkaline seawater.Operando Raman spectroscopy studies further identify structural changes of disorderedδ(NiIII-O)during the seawater oxidation process. | Longcheng Zhang Jie Liang Luchao Yue Kai Dong Jun Li Donglin Zhao Zerong Li Shengjun Sun Yongsong Luo Qian Liu Guanwei Cui Abdulmohsen Ali Alshehri Xiaodong Guo Xuping Sun | 2022 | Nano Research Energy2022，1，3： | 6 |
| 3 | Advancement toward Polymer Electrolyte Membrane Fuel Cells at Elevated Temperatures显示文摘Elevation of operational temperatures of polymer electrolyte membrane fuel cells(PEMFCs)has been demonstrated with phosphoric acid-doped polybenzimidazole(PA/PBI)membranes.The technical perspective of the technology is simplified construction and operation with possible integration with,e.g.,methanol reformers.Toward this target,significant efforts have been made to develop acid-base polymer membranes,inorganic proton conductors,and organic-inorganic composite materials.This report is devoted to updating the recent progress of the development particularly of acid-doped PBI,phosphate-based solid inorganic proton conductors,and their composite electrolytes.Long-term stability of PBI membranes has been well documented,however,at typical temperatures of 160℃.Inorganic proton-conducting materials,e.g.,alkali metal dihydrogen phosphates,heteropolyacids,tetravalent metal pyrophosphates,and phosphosilicates,exhibit significant proton conductivity at temperatures of up to 300℃ but have so far found limited applications in the form of thin films.Composite membranes of PBI and phosphates,particularly in situ formed phosphosilicates in the polymer matrix,showed exceptionally stable conductivity at temperatures well above 200℃.Fuel cell tests at up to 260℃ are reported operational with good tolerance of up to 16%CO in hydrogen,fast kinetics for direct methanol oxidation,and feasibility of nonprecious metal catalysts.The prospect and future exploration of new proton conductors based on phosphate immobilization and fuel cell technologies at temperatures above 200℃ are discussed. | Jin Zhang David Aili Shanfu Lu Qingfeng Li and San Ping Jiang | 2020 | Research2020，，1： | 6 |
| 4 | Electrodeposition of Pt-Decorated Ni(OH)_(2)/CeO_(2) Hybrid as Superior Bifunctional Electrocatalyst for Water Splitting显示文摘The facile synthesis of highly active and stable bifunctional electrocatalysts to catalyze water splitting is attractive but challenging.Herein,we report the electrodeposition of Pt-decorated Ni(OH)_(2)/CeO_(2)(PNC)hybrid as an efficient and robust bifunctional electrocatalyst.The graphite-supported PNC catalyst delivers superior hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities over the benchmark Pt/C and RuO_(2),respectively.For overall water electrolysis,the PNC hybrid only requires a cell voltage of 1.45V at 10mAcm-2 and sustains over 85 h at 1000mAcm^(-2).The remarkable HER/OER performances are attributed to the superhydrophilicity and multiple effects of PNC,in which Ni(OH)_(2)and CeO_(2)accelerate HER on Pt due to promoted water dissociation and strong electronic interaction,while the electron-pulling Ce cations facilitate the generation of high-valence Ni OER-active species.These results suggest the promising application of PNC for H2 production from water electrolysis. | Huanhuan Liu Zhenhua Yan Xiang Chen Jinhan Li Le Zhang Fangming Liu Guilan Fan Fangyi Cheng | 2020 | Research2020，，1： | 2 |
| 5 | Chemical hardness-driven interpretable machine learning approach for rapid search of photocatalysts显示文摘Strategies combining high-throughput(HT)and machine learning(ML)to accelerate the discovery of promising new materials have garnered immense attention in recent years.The knowledge of new guiding principles is usually scarce in such studies,essentially due to the‘black-box’nature of the ML models.Therefore,we devised an intuitive method of interpreting such opaque ML models through SHapley Additive exPlanations(SHAP)values and coupling them with the HT approach for finding efficient 2D watersplitting photocatalysts.We developed a new database of 30992D materials consisting of metals connected to six ligands in an octahedral geometry,termed as 2DO(octahedral 2D materials)database.The ML models were constructed using a combination of composition and chemical hardness-based features to gain insights into the thermodynamic and overall stabilities.Most importantly,it distinguished the target properties of the isocompositional 2DO materials differing in bond connectivities by combining the advantages of both elemental and structural features.The interpretable ML regression,classification,and data analysis lead to a new hypothesis that the highly stable 2DO materials follow the HSAB principle.The most stable 2DO materials were further screened based on suitable band gaps within the visible region and band alignments with respect to standard redox potentials using the GW method,resulting in 21 potential candidates.Moreover,HfSe_(2)and ZrSe_(2)were found to have high solar-tohydrogen efficiencies reaching their theoretical limits.The proposed methodology will enable materials scientists and engineers to formulate predictive models,which will be accurate,physically interpretable,transferable,and computationally tractable. | Ritesh Kumar Abhishek K.Singh | 2021 | npj Computational Materials2021，，1： | 0 |
| 6 | Two-dimensional oxide derived from high-temperature liquid metals via bubble templating显示文摘Two-dimensional(2D)oxide can be continuously produced by bubbling oxygen into liquid metals and the harvesting of these oxide relies on the proper choice of dispersion solvents.The mass-production of ligand-free 2D materials from high melting-point metals will not be possible if the limited stability of the traditional dispersion solvents is not circumvented.Herein,liquid tin was used for the first time in the bubbling protocol and 2D tin oxide was obtained in molten salts.The nanosheets were studied with combined microscopic and spectroscopic techniques,and high-density grain boundaries was identified between the sub-5-nm nano-crystallites in the nanosheets.It gives rise to the high performance in electrocatalytic CO_(2) reduction reaction.Density-functional-theory based calculation was applied to achieve a deeper understanding of the relationship between the activity,selectivity,and the grain-boundary features.The molten-salt based protocol could be explored for the synthesis of a library of functional 2D oxides. | Zheng Hu Tingbiao Yuan Hui Li Yishu Qiu Wei Zhou Jiangwei Zhang Yuxin Zhao Shi Hu | 2021 | Nano Research2021，14，12： | 0 |
| 7 | 一步法合成Fe_(2)P/Fe_(3)C@C双功能电催化剂用于高效析氢反应和析氧反应显示文摘开发高性能、低成本的双功能电催化剂用于大规模水电解仍是一个重大挑战.以六水合氯化铁(FeCl_(3)·6H_(2)O)、次磷酸钠(NaH_(2)PO_(2))、双氰胺(DCD)为原料通过一步固相烧结法合成出Fe_(2)P/Fe_(3)C@C.首先探讨了不同温度对样品结构和性能的影响,获得最佳的Fe_(2)P/Fe_(3)C@C(命名为Fe_(2)P/Fe_(3)C@C-800).然后通过X射线衍射仪(XRD)、显微共焦拉曼光谱仪(Raman)、扫描电子显微镜(SEM)、透射电子显微镜(TEM)与X射线光电子能谱仪(XPS)对Fe_(2)P/Fe_(3)C@C-800的组成、形貌以及微观结构等进行表征分析.另外,通过电催化测试表明,Fe_(2)P/Fe_(3)C@C-800催化剂在10 mA/cm2时碱性电解液中析氢反应和析氧反应的过电势分别为179 mV和245 mV,且分别能保持100 h和50 h的稳定性. | 张晓 黄剑锋 冯亮亮 曹丽云 | 2021 | 陕西科技大学学报2021，39，2： | 0 |
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