共查询到20条相似文献,搜索用时 15 毫秒
1.
Hao Xiong Chengfeng Du Zelin Ma Richeng Zhi Shuangshuang Hao Xiangyuan Zhao Zhe Liu Fei Xu Hongqiang Wang 《Advanced functional materials》2024,34(37):2402298
Electrocatalytic hydrogen evolution reaction (HER) via alkaline water splitting holds great promise for industrial clean hydrogen production but is frustrated by limited catalytic activity and inferior stability under high current density. Elaborate manipulating of heterostructure on robust catalytic electrodes is essential but challenging for accelerating HER kinetics with high durability. Herein, a robust nickel mesh electrode, offering high mechanical stability, is directly engineered with catalytic layers of multiple heterostructures (r-Mn–Ni/CoP) via facile one-pot electrodeposition followed by surface reconstruction strategy. The abundant heterostructures composed of crystalline CoP, NiP, amorphous region, and additional Mn doping considerably manipulate the electronic structure with optimized charge transfer; while the in situ surface-reconstructed hydrophilic nanoflakes enable the rapid wetting of active sites to the electrolyte. Consequently, the r-Mn–Ni/CoP requires only 134 mV overpotential at the current density of 100 mA cm−2, superior to monophasic and undoped samples, and the majority of reported HER catalysts. Remarkably, an electrolyzer with r-Mn–Ni/CoP on a nickel mesh cathode demonstrates extraordinary activity with a voltage of 1.734 V at 300 mA cm−2 and stable operation of 800 h. The finding provides a feasible strategy for the fabrication of nonprecious-metal-based HER electrocatalysts with high activity and stability toward industrial water electrolysis. 相似文献
2.
Yiwen Liao Guoxiong Deng Haoyu Wu Li Ding Haihui Wang 《Advanced functional materials》2024,34(3):2309871
Hydrogen energy is a truly renewable and clean energy source. Alkaline water electrolysis (AWE) is the most promising technology for green hydrogen production currently. In the AWE process, the critical part of an alkaline electrolyzer is the membrane, which acts to conduct hydroxide ions and block gases. However, developing low area resistance, high bubble point pressure and highly stable membrane for high-performance AWE is still a challenge. Herein, porous skeleton-supported composite membranes via the blade-coating method for advanced AWE are prepared. The porous composite membranes, besides having hydrophilic surface, also show ultra-low area resistance (≈0.15 Ω cm2), ultra-high bubble point pressure (≈27 bar) and excellent mechanical properties (tensile stress, ≈14 MPa). By using commercial catalysts, the composite membranes exhibit a current density of up to 1.9 A cm−2 at the voltage of 2 V in 30 wt% KOH solution at 80 °C and achieve ultra-high H2 purity (up to 99.996%) when applied in AWE. Notably, the composite membrane can operate for more than 1600 h without performance attenuation, demonstrating excellent stability. This study opens up the feasibility of preparing high-performance AWE membranes for large-scale hydrogen production. 相似文献
3.
Yan Wang;Ming Ni;Wei Yan;Chuhong Zhu;Daochuan Jiang;Yupeng Yuan;Haiwei Du; 《Advanced functional materials》2024,34(11):2311611
Electrocatalytic hydrogen production technology is essentially vital for future green and sustainable energy revolution while its large-scale industrial application is still unsatisfactory due to the low efficiency of electrocatalysts and kinetically sluggish oxygen evolution reaction (OER). Developing novel electrocatalysts and coupling them with upgrading organic molecules are considered effective solutions. Herein, it reports a high-entropy composite electrocatalyst consisting of FeCoNiAlMo alloy and carbon nanotube (CNT) for anodic benzyl alcohol (BA) electrooxidation coupled with cathodic hydrogen production. Because of the lower charge transfer resistance and faster reaction kinetics, the quinary FeCoNiAlMo/CNT is highly active to OER, remarkably outperforming the ternary FeCoNi/CNT counterpart. Then, the FeCoNiAlMo/CNT composite electrocatalyst is further utilized for BA oxidation reaction-assisted hydrogen evolution. Combining the experimental and calculation results, the different activities when tested in BA-containing or BA-free electrolytes can be attributed to the different metal active sites with specific surface adsorption effects to water and BA molecules, respectively. This work develops a novel electrocatalyst for high-efficient alcohol oxidation-assisted electrolysis. 相似文献
4.
N. Clament Sagaya Selvam Lijie Du Bao Yu Xia Pil J. Yoo Bo You 《Advanced functional materials》2021,31(12):2008190
Electroreduction of small molecules such as H2O, CO2, and N2 for producing clean fuels or valuable chemicals provides a sustainable approach to meet the increasing global energy demands and to alleviate the concern on climate change resulting from fossil fuel consumption. On the path to implement this purpose, however, several scientific hurdles remain, one of which is the low energy efficiency due to the sluggish kinetics of the paired oxygen evolution reaction (OER). In response, it is highly desirable to synthesize high-performance and cost-effective OER electrocatalysts. Recent advances have witnessed surface reconstruction engineering as a salient tool to significantly improve the catalytic performance of OER electrocatalysts. In this review, recent progress on the reconstructed OER electrocatalysts and future opportunities are discussed. A brief introduction of the fundamentals of OER and the experimental approaches for generating and characterizing the reconstructed active sites in OER nanocatalysts are given first, followed by an expanded discussion of recent advances on the reconstructed OER electrocatalysts with improved activities, with a particular emphasis on understanding the correlation between surface dynamics and activities. Finally, a prospect for clean future energy communities harnessing surface reconstruction-promoted electrochemical water oxidation will be provided. 相似文献
5.
Yansong Zhou Zhitong Wang Minghui Cui Haiyan Wu Yanjing Liu Qiongrong Ou Xinlong Tian Shuyu Zhang 《Advanced functional materials》2024,34(52):2410618
Developing high-efficiency alkaline water splitting technology holds great promise in potentially revolutionizing the traditional petrochemical industry to a more sustainable hydrogen economy. Importantly, the oxygen evolution reaction (OER) accompanied at the anode is considered as a critical bottleneck in terms of both complicated mechanism and sluggish kinetics, requiring rational design of OER electrocatalysts to elucidate the structure-performance relationship and reduce the applied overpotential. As a benchmarked non-precious metal candidate, NiFe-based electrocatalysts have gained enormous attention due to low-cost, earth-abundance, and remarkable intrinsic OER activity, which are expected to be implemented in industrial alkaline water splitting. In this contribution, a comprehensive overview of NiFe-based OER electrocatalysts is provided, starting with fundamental mechanisms, evaluation metrics, and synthetic protocols. Subsequently, basic principles with corresponding regulatory strategies are summarized following the sequence of substrate-catalyst-electrolyte design of efficient and robust NiFe-based electrocatalysts toward industrial-scale deployment. Perspectives on remaining challenges and instructive opportunities in this booming field are finally discussed. 相似文献
6.
Yitao Hu Li Shao Zhiqi Jiang Lei Shi Qiuju Li Kaiqian Shu Hui Chen Guodong Li Yan Dong Tongzhou Wang Jihong Li Lifang Jiao Yida Deng 《Advanced functional materials》2024,34(52):2411011
Urea oxidation reaction (UOR) is an ideal alternative to oxygen evolution reaction (OER) for efficient hydrogen production but is immensely plagued by slow kinetics. Herein, a multilayer hole amorphous boron-nickel catalyst (a-NiBx) is fabricated through a simple chemical plating method, which displays intriguing catalytic activity toward UOR, demanding a low working potential of 1.4 V to reach 100 mA cm−2. The high performance is credited to the formation of metaborate (BO2−), which can promote the formation of high-oxidation-state NiOOH active phase and optimize the adsorption of urea molecules. This can be confirmed by the operando spectroscopy characteristics and density functional theory calculations. Consequently, the assembled electrolyzer utilizing NiBx as bifunctional catalysts exhibited splendid catalytic activity, requiring an evidently lower voltage of 1.66 V to reach a current density of 100 mA cm−2 and 1.57 V when using Pt/C as a cathode catalyst. Moreover, the assembled electrolyzer secured a robust stability of over 200 h, as well as a four times higher hydrogen production rate than traditional water electrolysis. 相似文献
7.
Sanghwi Han;Jungwon Park;Jeyong Yoon; 《Advanced functional materials》2024,34(21):2314573
Developing high-performance and durable electrocatalysts for the oxygen evolution reaction (OER) is of utmost importance for green hydrogen production via anion exchange membrane water electrolysis (AEMWE). Herein, it is presented that a straightforward surface reconstruction strategy for preparing a robust Co-based OER catalyst with increased mass transfer activity while preserving the active CoOOH phase during the OER. This strategy comprises electrochemical oxidation of electrodeposited Co-based catalysts prior to heat treatment, allowing for the meticulous control of the oxidation potential to optimize the OER activity. The optimized catalyst exhibits an overpotential of 190 mV at 10 mA cm−2 and a Tafel slope of 32.7 mV dec−1 under half-cell conditions. In an AEMWE single-cell system, it shows a current density of 1590 mA cm−2 at 1.8 V and 60 °C and demonstrates a degradation rate of 0.2 mV h−1 during 1000 h of operation at 500 mA cm−2. This study not only provides a simple yet potent strategy to enhance the OER activity but also offers insights regarding the factors enhancing the OER performance. 相似文献
8.
Lei Zhang Sang‐Il Choi Jing Tao Hsin‐Chieh Peng Shuifen Xie Yimei Zhu Zhaoxiong Xie Younan Xia 《Advanced functional materials》2014,24(47):7520-7529
This article reports a facile synthesis of Pd‐Cu bimetallic tripods with a purity over 90%. Two requirements must be met in order to form tripods: i) formation of triangular, plate‐like seeds during the nucleation step and ii) preferential deposition of atoms onto the three corners of a seed during the growth step. In this synthesis, these requirements are fulfilled by adding CuCl2 and KBr into an aqueous synthesis. Specifically, it is demonstrated that the Cu atoms resulting from underpotential deposition could greatly reduce the energy barrier involved in the formation of triangular seeds with planar defects because of the much lower stacking fault energy (41 mJ·m?2 for Cu vs 220 mJ·m?2 for Pd). The Br? ions could strongly bind to the three {100} side faces of a triangular seed, forcing the Pd atoms to grow from the three corners of a seed to generate a tripod. When compared with commercial Pd black, the Pd‐Cu tripods exhibited substantially enhanced catalytic activity toward the electro‐oxidation of formic acid. This work offers a general strategy for the synthesis of nanocrystals with a tripod structure for catalytic applications. 相似文献
9.
Yi-Ming Liu Bo-Qiang Miao Han-Yue Yang Xuan Ai Tian-Jiao Wang Feng Shi Pei Chen Yu Chen 《Advanced functional materials》2024,34(38):2402485
The rational design of the electronic structure and elemental compositions of anode electrocatalysts for formic acid electrooxidation reaction (FAOR) is paramount for realizing high-performance direct formic acid fuel cells. Herein, palladium-boride nanoflowers (Pd-B NFs) with controllable boron content are rationally designed via a simple wet chemical reduction method, utilizing PdII-dimethylglyoxime as precursor and NaBH4 as both reductant and boron source. The boron content of Pd-B NFs can be regulated through manipulation of reaction time, accompanying with the crystal phase transition from face-centered cubic to hexagonal close-packed within the parent Pd lattice. The obtained Pd-B NFs exhibit increased FAOR mass and specific activity with increasing boron content, showcasing remarkable inherent stability and anti-poisoning capability compare to commercial Pd and platinum (Pt) nanocrystals. Notably, the sample reacted for 12 h reveals high FAOR specific activity (31.5 A m−2), which is approximately two times higher than the commercial Pd nanocrystals. Density functional theory calculations disclose that the d-sp orbital hybridization between Pd and B modifies surface d-band properties of Pd, thereby optimizing the adsorption of key intermediates and facilitating FAOR kinetics on the Pd surface. This study paves the way toward the utilization of metal boride-based materials with simple synthesis methods for various electrocatalysis applications. 相似文献
10.
Yingjun Sun Weibin Chen Wenshu Zhang Yan Nie Qinghua Zhang Lin Gu Mingchuan Luo Shaojun Guo 《Advanced functional materials》2023,33(31):2303299
Spreading the formic acid (HCOOH) fuel cells demands a better anode electrocatalyst for the oxidation of formic acid. The catalytic efficiency of platinum (Pt)– the only choice of practicability, is mainly limited by its intrinsic affinity to CO, thus desiring a proper release. Herein, theoretical calculations are first leveraged to find that the introduction of iridium (Ir) can facilitate HCOOH oxidation with robust CO tolerance through a dehydrogenation pathway. Then, this strategy experimentally by designing a new trimetallic catalyst of 2D porous PtIrBi nanoplates (p-PtIrBi NPs) is implemented. The optimized p-PtIrBi NPs/C exhibits a very high mass activity of 8.2 A mg−1pt and a high retention rate of 55.9% after the durability test, which is among the best formic acid oxidation catalysts reported to date, much higher than those of PtIrBi NPs/C, PtBi NPs/C, and Pt/C. The CO-stripping and in situ Fourier transform infrared (FTIR) experiments collectively evidence that two types of due site, i.e., “Pt-Bi” and “Ir-Bi”, endow the catalyst with suppressed CO-poisoning property to achieve super-high activity and stability for formic acid oxidation reaction. 相似文献
11.
Zihan Ma Xiaofei Lu Sunghyun Park Tatsuya Shinagawa Masashi Okubo Kazuhiro Takanabe Atsuo Yamada 《Advanced functional materials》2023,33(25):2214466
Hydrogen is a promising alternative to fossil fuels that can reduce greenhouse gas emissions. Decoupled water electrolysis system using a reversible proton storage redox mediator, where the oxygen evolution reaction and hydrogen evolution reaction are separated in time and space, is an effective approach to producing hydrogen gas with high purity, high flexibility, and low cost. To realize fast hydrogen production in such a system, a redox mediator capable of releasing protons rapidly is required. Herein, α-MoO3, with an ultrafast proton transfer property that can be explained by a dense hydrogen bond network in the lattice oxygen arrays of HxMoO3, is examined as a high-rate redox mediator for fast hydrogen production in acidic electrolytes. The α-MoO3 redox mediator shows both a large capacity of 204 mAh g−1 and fast hydrogen production at a current rate of 10 A cm−2(≈153 A g−1), outperforming most of the previously reported solid-state redox mediators. 相似文献
12.
以嗜碱芽胞杆菌BC -A3 6为出发菌株,通过紫外线(UV)、亚硝基胍(NTG)及激光复合诱变处理,选育出一株目前高产碱性淀粉酶的突变株JG -5 7,在摇瓶发酵培养基上3 5℃培养45h ,测得酶活力稳定在867u/ml左右,为出发菌株酶活力的2 .1倍。该菌株产酶适宜的pH值为9-10。 相似文献
13.
Wenxia Chen Wei Wei Fan Li Yujie Wang Meng Liu Shuai Dong Jinhai Cui Yongya Zhang Rui Wang Kostya Ostrikov Shuang-Quan Zang 《Advanced functional materials》2024,34(7):2310690
The development of bifunctional electrocatalysts suitable for a wide pH range and seawater splitting under simulated industrial electrolysis conditions is expected to advance practical applications of clean hydrogen energy. Here, the study reports a built-in electric field approach to assemble heterogeneous Ru nanoclusters (Ru NCs) anchored in P,O co-doped NiFe layered double hydroxide bifunctional electrocatalysts (Ru NCs/P,O-NiFe LDH) for overall water splitting. It is revealed that the BEF ensures electron enrichment via unidirectional electron transfer from P,O-NiFe LDH to Ru nanoclusters due to the difference in the corresponding Fermi levels. The optimized Ru NCs/P,O-NiFe LDH/NF shows excellent electrocatalytic activity toward hydrogen evolution reaction, oxygen evolution reaction, and overall water splitting in a wide pH range, as well as simulated seawater electrolysis under industry-relevant conditions. The long-term catalyst stability under high currents and industrial process temperatures is also demonstrated. Density functional theory calculations further confirm that the active sites at the BEF interface effectively reduce the energy barrier of water electrolysis, thereby facilitating the electrocatalytic processes. 相似文献
14.
Pu Zhang Han Man Yao Huo Fei Zhang Yang Liu Renbing Wu Fei Wang Dalin Sun 《Advanced functional materials》2024,34(49):2409365
The development of efficient and long-term stable electrodes for hydrogen evolution reaction (HER) in seawater is highly desirable for hydrogen generation but remains challenging. In this work, a highly active CrOx@Ni2P-Ni5P4/NF electrode is developed and investigated its dynamic reconstruction for HER in neutral electrolytes. The combination of in situ Raman spectra and electrochemical measurements revealed the dynamic surface reconstruction of the catalyst during HER. The CrOx modification not only effectively facilitates water dissociation but also stabilizes the structure post-reconstruction, enabling rapid and stable hydrogen generation in neutral media. Remarkably, CrOx@Ni2P-Ni5P4/NF exhibits overpotentials of 109 and 263 mV at current densities of 10 and 100 mA cm−2 in 1 m PBS, respectively. Concurrently, it exhibits stable operation for 500 h in 1 m PBS and 140 h in natural seawater at current densities of 50 and 100 mA cm−2, respectively. The proposed catalytic electrode and the mechanistic insights present a significant stride toward the realization of metal phosphides for direct seawater splitting. 相似文献
15.
利用微波辅助有机溶胶法成功制备了Pd3Ru/C纳米电催化剂。相比传统的高压有机溶胶法,该法大大降低了有机溶剂的使用量并缩减了反应时间,是一种环境友好和资源节约的新型方法。采用XRD,TEM,XPS和电化学测试等手段对其结构和电化学性能进行了表征和评价。XRD和TEM结果表明微波辅助制备的Pd3Ru/C催化剂其粒径只有约3.0 nm,分散性也较Pd/C得到显著改善;XPS谱图证实催化剂活性组分Pd和Ru的原子比约为3.13∶1,Pd和Ru两种元素间发生了相互作用。与同条件制备的Pd/C催化剂相比,Pd3Ru/C催化剂在电极上发生甲酸氧化反应的主要峰电位负移了约100 mV,峰电流密度增大了2/3左右,其甲酸电氧化活性得到明显提高。 相似文献
16.
Songhu Bi Zhen Geng Yuwei Wang Zijian Gao Liming Jin Mingzhe Xue Cunman Zhang 《Advanced functional materials》2023,33(31):2214792
Alkaline water electrolysis (AWE) is the promising technical pathway of large-scale green hydrogen production. The sluggish oxygen evolution reaction seriously hampers the water decomposition reaction kinetics for AWE, especially at high current density above 500 mA cm−2. It is closely related with bubbles removal dynamic performance of porous electrodes. In this study, the multi-stage porous nickel–iron oxide electrode is prepared by a two-step electro-deposition method. The electrode shows good oxygen evolution reaction performance at high current densitiy of 1000 mA cm−2, which is attributed to both the good electro-catalytic performance of NiFeOx with nano-cone structure and good bubbles removal performance of porous Ni interlayer with the curved pore channels. Bubbles motion inside the pore channels is deeply analyzed by Lattice Boltzmann simulation of gas–liquid two-phase flows, combining with the experiments. The results indicate that bubbles motion speed is faster in curved pore channels than that in straight pore channels due to the role of bubble buoyancy. It illuminates the effects of pore channel curvature on bubbles motion for porous electrodes prepared by electro-deposition. It provides the possibility of designing porous electrodes with both good electro-catalytic performance and good bubbles removal performance by the electro-deposition method, from the view of industrial applications. 相似文献
17.
发射率是一项重要的表征物体表面辐射特性的热物性参数,与温度、测量波长、表面氧化、表面粗糙度等多种因素相关,研究其变化特征对红外测量有着重要意义。本文研究了在大气条件下,温度为800~1160 K范围内,测量波长为1.5 μm,带宽20 nm,钢SPHC样品的氧化特性对光谱发射率的影响。实验中每隔40 K为一个温度测量点,样品达到测量温度,持续加热3 h以上,每隔5 min记录一次光谱发射率的值。实验结果表明:①在相对低温阶段800 K、840 K铁与氧气生成三氧化二铁,该温度下氧化膜的增长主要来自这一反应过程;②在960 K左右三氧化二铁与铁反应生成氧化亚铁,这一阶段在测量温度下缓慢进行,需要较长时间样品表面光谱发射率才趋于稳定;③在1120 K以上,光谱发射率基本保持不变,样品表面氧化亚铁氧化膜快速形成。另一方面,我们拟合了在相同的加热时间里,温度对光谱发射率的影响,得出不同加热时间下温度与发射率之间的关系模型与实际模型之间描述非常准确一致。最后,实际应用中,在测量钢铁的温度时,应充分考虑由于空气中表面氧化对光谱发射率带来的影响。 相似文献
18.
Xiaoyu Qiu Hanyue Zhang Peishan Wu Fengqi Zhang Shaohua Wei Dongmei Sun Lin Xu Yawen Tang 《Advanced functional materials》2017,27(1)
Freestanding ultrathin 2D noble metal nanosheets have drawn enormous attention due to their potential applications in various fields. However, the synthesis of 2D noble metal nanosheets still remains a great challenge due to the lack of an intrinsic driving force for anisotropic growth of 2D structures. Here, a facile one‐pot synthesis of ultrathin freestanding porous Pd nanosheets (≈2.5 µm in lateral size and 10 nm in thickness) flexibly knitted by interweaved ultrathin nanowires with the assistance of poly(diallyldimethylammonium chloride) is presented. Nanoparticles attachment and subsequent self‐assembly in the synthetic process are responsible for the formation of such intriguing nanostructures. Moreover, finely controlling the pH value of the precursor solution leads to yield different Pd nanostructures with tunable dimensionalities, including 3D nanoflowers, 2D nanosheets, and 1D nanochains. Owing to the unique structural features, the obtained freestanding porous Pd nanosheets exhibit excellent electrocatalytic activity and stability towards formic acid oxidation compared to those of other dimensional counterparts and commercial Pd black. 相似文献
19.
Yu Liao Yangyang Chen Lei Li Sha Luo Yan Qing Cuihua Tian Han Xu Jingxian Zhang Yiqiang Wu 《Advanced functional materials》2023,33(42):2303300
Constructing effective electrocatalysts based on ultrafine heterostructures is a promising strategy for boosting catalytic performance by exposing active sites and increasing specific surface area. However, the fabrication of catalytically active heterostructures with elaborate architectures is still poorly developed owing to synthetic challenges, and the intrinsic mechanism of heterogeneous interfaces remains unclear because of insufficient evidence regarding real active sites. In this study, ultrafine homologous Ni2P–Co2P heterostructures (Ni2P–Co2P/C) are created using a topological transformation strategy from a Ni–Co layered double hydroxide/carbon (Ni–Co LDH/C) interconnected structure in a single nanosheet. When employed as catalysts in urea oxidation reaction (UOR), the Ni2P–Co2P/C heterostructures exhibit superior activity and stability, attributed to the optimized geometric and electronic structures of the catalytic sites. Specifically, it takes an ultralow potential of 1.27 V to reach a current density of 10 mA cm−2 with a small Tafel slope of 28.71 mV dec−1. The operando analyses and calculation results reveal that cobalt incorporation can reduce the generation potential of the surface reconstructive active species and optimize the absorption/desorption energy of the intermediates. Overall, this study proposes an efficient and cost-effective UOR electrocatalyst and offers a new high-performance homologous heterostructure design for widespread application. 相似文献
20.
碱性淀粉酶菌株的紫外线和He-Ne激光复合诱变的研究 总被引:1,自引:2,他引:1
以嗜碱芽胞杆菌(alkaliphilic bacillus)BC-A36为出发菌株,通过紫外线,N-甲基-N′-硝基-亚硝基胍(亚硝基胍NTG)和激光复合诱变处理,选育出一株高产碱性淀粉酶的突变株JG-57,在摇瓶发酵培养基上35~37℃培养45 h,测得酶活力稳定在867 u/mL左右,为出发菌株酶活力的2.1倍。该突变株产酶温度在25~43℃,最适温度37℃,产酶pH值7~12,最适pH值9。该酶较稳定的pH值适宜范围为9.5~10。传代实验证明,该突变株遗传性能稳定。说明激光辐照是碱性淀粉酶菌株有效的选育方法。该突变株产生的碱性淀粉酶可适用于淀粉的液化、洗涤及纺织工业等。 相似文献