一步法合成的FeOOH/黑磷纳米复合材料协同实现体系优异的析氧性能

通过水热法,在黑磷(BP)纳米片表面生长FeOOH纳米材料,制备出FeOOH/BP纳米复合材料。作为电化学析氧反应(OER)催化剂,该复合材料在20 mA·cm^-2时的过电位仅为191 mV,Tafel斜率为49.9 mV dec^-1;在循环1 000圈后,过电位仅仅增加了3 mV,且循环过程中元素价态不变,表现出优秀的稳定性。纳米FeOOH负载于BP表面,客观上能隔断氧气对BP的氧化,保护BP的载流子传导性能。同时,生长的FeOOH颗粒尺度小,结晶性弱,这有利于丰富其活性位点,增大活性面积。     

一步法合成的FeOOH/黑磷纳米复合材料协同实现体系优异的析氧性能

通过水热法，在黑磷(BP)纳米片表面生长FeOOH纳米材料，制备出FeOOH/BP纳米复合材料。作为电化学析氧反应(OER)催化剂，该复合材料在20 mA·cm^-2时的过电位仅为191 mV，Tafel斜率为49.9 mV dec^-1；在循环1 000圈后，过电位仅仅增加了3 mV，且循环过程中元素价态不变，表现出优秀的稳定性。纳米FeOOH负载于BP表面，客观上能隔断氧气对BP的氧化，保护BP的载流子传导性能。同时，生长的FeOOH颗粒尺度小，结晶性弱，这有利于丰富其活性位点，增大活性面积。     

NiFe水滑石纳米片阵列负载Ru用于提升碱性电催化析氢和析氧性能

通过离子交换的方式将Ru负载到NiFe水滑石(LDH)纳米阵列表面得到(Ru/NiFe LDH),Ru的引入显著提升了NiFe LDH的活性比表面积,暴露了更多的活性位点,同时调控了其电子结构,大大提升了其本征催化活性。在碱性条件下,催化析氢反应时仅需50 mV的过电位即可达到10 mA·cm^-2的电流密度,Tafel斜率为52.3 mV·dec^-1。而相同条件下原始NiFe LDH达到10mA·cm^-2的电流密度则需要226 mV的过电位,Tafel斜率为157.5 mV·dec^-1。同时制备的Ru/NiFe LDH也展现出了良好的析氧催化活性,在50 mA·cm^-2的电流密度下,过电位仅为231 mV,而NiFe LDH则需237 mV。Ru/NiFe LDH在长时间的电催化条件下依然能保持良好的工作稳定性。     

MoSe2/Co-MOF/NF复合材料的制备及电催化产氧性能

设计高效的催化剂对于电解水制氢至关重要。基于过渡金属硒化物(TMSe)的高催化活性和金属有机骨架(MOFs)的灵活结构,我们提出了一种将MOFs与TMSe复合的策略,在导电基底泡沫镍(NF)上生长的复合材料不仅继承了2种单体的优点,还有效地改善了MOFs导电性差、TMSe易团聚的缺点。MoSe₂/Co-MOF/NF在碱性溶液中展示出优异的电催化产氧活性,在电流密度为10 mA·cm^-2时其过电位仅为242 mV,塔菲尔斜率仅为50.64 mV·dec^-1。此外,该材料在碱性溶液中经1 000圈循环伏安(CV)循环测试和30 h的恒电压电解测试均表现出良好的稳定性。     

MoSe2/Co-MOF/NF复合材料的制备及电催化产氧性能

设计高效的催化剂对于电解水制氢至关重要。基于过渡金属硒化物(TMSe)的高催化活性和金属有机骨架(MOFs)的灵活结构，我们提出了一种将MOFs与TMSe复合的策略，在导电基底泡沫镍(NF)上生长的复合材料不仅继承了2种单体的优点，还有效地改善了MOFs导电性差、TMSe易团聚的缺点。MoSe₂/Co-MOF/NF在碱性溶液中展示出优异的电催化产氧活性，在电流密度为10 mA·cm^-2时其过电位仅为242 mV，塔菲尔斜率仅为50.64 mV·dec^-1。此外，该材料在碱性溶液中经1 000圈循环伏安(CV)循环测试和30 h的恒电压电解测试均表现出良好的稳定性。     

CoFeOx/MoO2准平行纳米阵列电极的析氢性能

利用CoFe层状双金属氢氧化物(CoFe LDH)准平行纳米片阵列作为载体前驱体,通过原位负载及煅烧方式,实现了含有氧空位的 MoO₂纳米颗粒在纳米片阵列表面的生长。电化学研究结果表明,所得 CoFeO_x/MoO₂纳米阵列电极具有高析氢反应(HER)催化活性。该电极在10和1 000 mA·cm^-2时的HER过电位分别为40和217 mV。在50 mA·cm^-2的电流密度下,该电极可以稳定运行125 h。     

NiFe水滑石纳米片阵列负载Ru用于提升碱性电催化析氢和析氧性能

通过离子交换的方式将Ru负载到NiFe水滑石（LDH）纳米阵列表面得到（Ru/NiFe LDH），Ru的引入显著提升了NiFe LDH的活性比表面积，暴露了更多的活性位点，同时调控了其电子结构，大大提升了其本征催化活性。在碱性条件下，催化析氢反应时仅需50 mV的过电位即可达到10 mA·cm^-2的电流密度，Tafel斜率为52.3 mV·dec^-1。而相同条件下原始NiFe LDH达到10mA·cm^-2的电流密度则需要226 mV的过电位，Tafel斜率为157.5 mV·dec^-1。同时制备的Ru/NiFe LDH也展现出了良好的析氧催化活性，在50 mA·cm^-2的电流密度下，过电位仅为231 mV，而NiFe LDH则需237 mV。Ru/NiFe LDH在长时间的电催化条件下依然能保持良好的工作稳定性。     

两步电沉积构建NiFe/Ni3S2/NF分级异质电极用于大电流密度析氧反应

通过简便的两步电沉积法在泡沫镍表面有效复合非晶态Ni₃S₂材料与富缺陷的NiFe双金属羟基氧化物,从而构建了NiFe/Ni₃S₂/NF三维分级纳米异质电极。受益于非晶态Ni₃S₂和富缺陷NiFe材料的结构和催化优势,以及异质界面的强电子相互作用,使得NiFe/Ni₃S₂/NF催化电极表现出优异的析氧催化性能：达到100 mA·cm^-2时的析氧过电位仅为273 mV,远优于大多数已报道的Ni/Fe基复合材料。值得注意的是,在1 mol·L^-1 KOH溶液中,仅需~372 mV的过电位即可稳定输出1 000 mA·cm^-2的高电流密度达27 h以上。     

石墨烯负载Ni2P纳米片作为锂硫电池的硫基复合正极材料

将磷化镍纳米片均匀负载到石墨烯(G)上制备出Ni₂P/G复合材料,并将其作为硫载体构筑了硫基复合材料(S/Ni₂P/G)。研究表明,磷化镍纳米片对可溶性多硫化物具有强的化学作用和较高的电催化活性,使S/Ni₂P/G硫基复合材料表现出良好的电化学性能。特别是,在高硫含量(80.3%)和低电解液用量(15μL·mg^-1)条件下,S/Ni₂P/G硫基复合材料展现出1 164.7mAh·g^-1的质量比容量和良好的循环稳定性。此外,S/Ni₂P/G复合材料具有高的振实密度(1.02 g·cm^-3),其体积比容量高达954.0mAh·cm^-3,约为S/G复合材料体积比容量的1.6倍。     

NiO/MnO2分级纳米片阵列复合材料的制备与超电容性能

通过化学浴沉积和水热法在泡沫镍上制备了NiO/MnO₂分级纳米片阵列复合材料,XRD和SEM测试表明NiO纳米片垂直生长在泡沫镍上,交叉形成网状阵列结构;MnO₂纳米介孔泡沫进一步生长在NiO纳米片两侧,与NiO形成了壳核式的复合结构。循环伏安和恒流充放电测试发现,NiO/MnO₂分级纳米片阵列复合材料的电化学性能相比复合前得到明显改善,在1 A·g^-1的电流密度下,比电容提高至1 297 F·g^-1;2 A·g^-1下循环1 000次,比电容保持率高达97%,比电容和循环性能的改善是由于分级纳米片阵列复合结构方便了电解液传质,扩大了活性材料与电解液的接触,促进了赝电容反应,提高了NiO和MnO₂的结构稳定性。     

Interface‐Engineered Ni(OH)2/β‐like FeOOH Electrocatalysts for Highly Efficient and Stable Oxygen Evolution Reaction

Iron‐based (oxy)hydroxides are especially attractive electrocatalysts for the oxygen evolution reaction (OER) owing to their earth abundance, low cost, and nontoxicity. However, poor OER kinetics on the surface restricts the performance of the FeOOH electrocatalyst. Herein, a highly efficient and stable Ni(OH)₂/β‐like FeOOH electrocatalyst is obtained by facile electroactivation treatment. The activated Ni(OH)₂/β‐like FeOOH sample indicates an overpotential of 300 mV at 10 mA cm⁻² for the OER, and no clear current decay after 50 h of testing; this is comparable to the most efficient nickel‐ and cobalt‐based electrocatalysts on planar substrates. Furthermore, studies suggest that β‐like FeOOH plays a key role in remarkably enhancing the performance during the electroactivation process owing to its metastable tunnel structure with a lower barrier for interface diffusion of Ni²⁺ ions between the bilayer electrocatalyst. This study develops a new strategy to explore efficient and low‐cost electrocatalysts and deepens understanding of bilayer electrocatalysts for the OER.     

Strong‐Coupled Cobalt Borate Nanosheets/Graphene Hybrid as Electrocatalyst for Water Oxidation Under Both Alkaline and Neutral Conditions

Developing highly active catalysts for the oxygen evolution reaction (OER) is of paramount importance for designing various renewable energy storage and conversion devices. Herein, we report the synthesis of a category of Co‐Pi analogue, namely cobalt‐based borate (Co‐B_i) ultrathin nanosheets/graphene hybrid by a room‐temperature synthesis approach. Benefiting from the high surface active sites exposure yield, enhanced electron transfer capacity, and strong synergetic coupled effect, this Co‐B_i NS/G hybrid shows high catalytic activity with current density of 10 mA cm^?2 at overpotential of 290 mV and Tafel slope of 53 mV dec^?1 in alkaline medium. Moreover, Co‐B_i NS/G electrocatalysts also exhibit promising performance under neutral conditions, with a low onset potential of 235 mV and high current density of 14.4 mA cm^?2 at 1.8 V, which is the best OER performance among well‐developed Co‐based OER electrocatalysts to date. Our finding paves a way to develop highly active OER electrocatalysts.     

一种家蚕茧衍生具有蜂窝状结构的钴-锰共掺杂碳材料双功能电解水催化剂

通过一步碳化石墨化过程,由家蚕茧制得了一种具有蜂窝状结构的氮钴锰共掺杂碳材料。该材料具有蜂窝状结构和高比表面积,同时由于暴露的钴-锰活性位点以及富含的吡啶氮和石墨氮,3%钴-锰/蚕茧的碳材料(3%Co-Mn/SCC)显示了高析氢反应活性,其初始电位和10 m A·cm~(-2)过电位分别只有121和155 m V,Tafel斜率为130 m V·dec~(-1),并且在酸性条件下具有很好的稳定性。与此同时,2%Co-Mn/SCC在碱性条件下表现出优异的析氧反应催化性能,具有较低的初始电位,Tafel斜率为143 m V·dec~(-1)。     

Bimetallic Metal‐Organic Framework‐Derived Nanosheet‐Assembled Nanoflower Electrocatalysts for Efficient Oxygen Evolution Reaction

Non‐noble metal‐based metal–organic framework (MOF)‐derived electrocatalysts have recently attracted great interest in the oxygen evolution reaction (OER). Here we report a facile synthesis of nickel‐based bimetallic electrocatalysts derived from 2D nanosheet‐assembled nanoflower‐like MOFs. The optimized morphologies and large Brunauer–Emmett–Teller (BET) surface area endow FeNi@CNF with efficient OER performance, where the aligned nanosheets can expose abundant active sites and benefit electron transfer. The complex nanoflower morphologies together with the synergistic effects between two metals attributed to the OER activity of the Ni‐based bimetallic catalysts. The optimized FeNi@CNF afforded an overpotential of 356 mV at a current density of 10 mA cm^?2 with a Tafel slope of 62.6 mV dec^?1, and also exhibited superior durability with only slightly degradation after 24 hours of continuous operation. The results may inspire the use of complex nanosheet‐assembled nanostructures to explore highly active catalysts for various applications.     

泡沫镍原位负载双金属AlCo层状双氢氧化物纳米催化剂高效电催化析氧反应

经一步水热法在泡沫镍（NF）上原位生长获得了AlCo-LDH/NF （LDH=层状双氢氧化物）催化剂。基于AlCo-LDH的高表面积和良好相界面,催化剂表现出了优异的电催化析氧反应（OER）活性。在碱性介质中,当电流密度为200 mA·cm^-2时,AlCo₃-LDH/NF催化剂具有419 mV的低过电位和50.04 mV·dec^-1的低Tafel斜率。     

简易电沉积法制备CoFe-P催化剂用于高效析氧反应

开发低成本、高活性且稳定的非贵金属催化剂是实现大规模电解水制氢的关键所在。在此,我们通过简便、合理的电沉积法在泡沫镍(NF)上构建了一种具备超薄二维纳米片形貌的高度非晶相Co1Fe1-P薄膜用于高效催化析氧反应（OER）。在1.0mol·L^-1 KOH溶液中,所制备的Co1Fe1-P/NF催化剂在电流密度为10和100 mA·cm^-2处的过电位分别为274.4和329.5 mV,Tafel斜率仅为45.3 mV·dec^-1,可以媲美商业RuO₂催化剂。此外,Co1Fe1-P/NF催化剂在10 mA·cm^-2的100 h计时电压法测试和1 000次循环伏安法测试中均表现出卓越的催化稳定性。Co1Fe1-P/NF催化剂优秀的催化活性归因于其独特的形貌、高度非晶相结构提供的低能垒、优化的电子结构以及钴磷化物和铁磷化物的强协同效应。     

简易电沉积法制备CoFe-P催化剂用于高效析氧反应

开发低成本、高活性且稳定的非贵金属催化剂是实现大规模电解水制氢的关键所在。在此,我们通过简便、合理的电沉积法在泡沫镍(NF)上构建了一种具备超薄二维纳米片形貌的高度非晶相Co1Fe1-P薄膜用于高效催化析氧反应(OER)。在1.0mol·L^-1 KOH溶液中,所制备的Co1Fe1-P/NF催化剂在电流密度为10和100 mA·cm^-2处的过电位分别为274.4和329.5 mV,Tafel斜率仅为 45.3 mV·dec^-1,可以媲美商业 RuO₂催化剂。此外,Co1Fe1-P/NF 催化剂在 10 mA·cm^-2的 100 h 计时电压法测试和1 000次循环伏安法测试中均表现出卓越的催化稳定性。Co1Fe1-P/NF催化剂优秀的催化活性归因于其独特的形貌、高度非晶相结构提供的低能垒、优化的电子结构以及钴磷化物和铁磷化物的强协同效应。     

Coupling of Bifunctional CoMn‐Layered Double Hydroxide@Graphitic C3N4 Nanohybrids towards Efficient Photoelectrochemical Overall Water Splitting

The development of durable, low‐cost, and efficient photo‐/electrolysis for the oxygen and hydrogen evolution reactions (OER and HER) is important to fulfill increasing energy requirements. Herein, highly efficient and active photo‐/electrochemical catalysts, that is, CoMn‐LDH@g‐C₃N₄ hybrids, have been synthesized successfully through a facile in situ co‐precipitation method at room temperature. The CoMn‐LDH@g‐C₃N₄ composite exhibits an obvious OER electrocatalytic performance with a current density of 40 mA cm^?2 at an overpotential of 350 mV for water oxidation, which is 2.5 times higher than pure CoMn‐LDH nanosheets. For HER, CoMn‐LDH@g‐C₃N₄ (η₅₀=?448 mV) requires a potential close to Pt/C (η₅₀=?416 mV) to reach a current density of 50 mA cm². Furthermore, under visible‐light irradiation, the photocurrent density of the CoMn‐LDH@g‐C₃N₄ composite is 0.227 mA cm^?2, which is 2.1 and 3.8 time higher than pristine CoMn‐LDH (0.108 mA cm^?2) and g‐C₃N₄ (0.061 mA cm^?2), respectively. The CoMn‐LDH@g‐C₃N₄ composite delivers a current density of 10 mA cm^?2 at 1.56 V and 100 mA cm^?2 at 1.82 V for the overall water‐splitting reaction. Therefore, this work establishes the first example of pure CoMn‐LDH and CoMn‐LDH@g‐C₃N₄ hybrids as electrochemical and photoelectrochemical water‐splitting systems for both OER and HER, which may open a pathway to develop and explore other LDH and g‐C₃N₄ nanosheets as efficient catalysts for renewable energy applications.