共查询到20条相似文献,搜索用时 0 毫秒
1.
Dr. Hongmei Gao Dr. Zhaohui Xiao Shiqian Du Dr. Tianyang Liu Dr. Yu-Cheng Huang Jianqiao Shi Yanwei Zhu Gen Huang Bo Zhou Yongmin He Prof. Chung-Li Dong Prof. Yafei Li Prof. Ru Chen Prof. Shuangyin Wang 《Angewandte Chemie (International ed. in English)》2023,62(49):e202313954
Due to the robust oxidation conditions in strong acid oxygen evolution reaction (OER), developing an OER electrocatalyst with high efficiency remains challenging in polymer electrolyte membrane (PEM) water electrolyzer. Recent theoretical research suggested that reducing the coordination number of Ir−O is feasible to reduce the energy barrier of the rate-determination step, potentially accelerating the OER. Inspired by this, we experimentally verified the Ir−O coordination number's role at model catalysts, then synthesized low-coordinated IrOx nanoparticles toward a durable PEM water electrolyzer. We first conducted model studies on commercial rutile-IrO2 using plasma-based defect engineering. The combined in situ X-ray absorption spectroscopy (XAS) analysis and computational studies clarify why the decreased coordination numbers increase catalytic activity. Next, under the model studies’ guidelines, we explored a low-coordinated Ir-based catalyst with a lower overpotential of 231 mV@10 mA cm−2 accompanied by long durability (100 h) in an acidic OER. Finally, the assembled PEM water electrolyzer delivers a low voltage (1.72 V@1 A cm−2) as well as excellent stability exceeding 1200 h (@1 A cm−2) without obvious decay. This work provides a unique insight into the role of coordination numbers, paving the way for designing Ir-based catalysts for PEM water electrolyzers. 相似文献
2.
Jing Zhang Yufeng Zhao Wanting Zhao Jing Wang Yongfeng Hu Chengyu Huang Xingli Zou Yang Liu Dengsong Zhang Xionggang Lu Hongjin Fan Yanglong Hou 《Angewandte Chemie (International ed. in English)》2023,62(52):e202314303
Transition metal single atom electrocatalysts (SACs) with metal-nitrogen-carbon (M−N−C) configuration show great potential in oxygen evolution reaction (OER), whereby the spin-dependent electrons must be allowed to transfer along reactants (OH−/H2O, singlet spin state) and products (O2, triplet spin state). Therefore, it is imperative to modulate the spin configuration in M−N−C to enhance the spin-sensitive OER energetics, which however remains a significant challenge. Herein, we report a local field distortion induced intermediate to low spin transition by introducing a main-group element (Mg) into the Fe−N−C architecture, and decode the underlying origin of the enhanced OER activity. We unveil that, the large ionic radii mismatch between Mg2+ and Fe2+ can cause a FeN4 in-plane square local field deformation, which triggers a favorable spin transition of Fe2+ from intermediate (dxy2dxz2dyz1dz21, 2.96 μB) to low spin (dxy2dxz2dyz2, 0.95 μB), and consequently regulate the thermodyna-mics of the elementary step with desired Gibbs free energies. The as-obtained Mg/Fe dual-site catalyst demonstrates a superior OER activity with an overpotential of 224 mV at 10 mA cm−2 and an electrolysis voltage of only 1.542 V at 10 mA cm−2 in the overall water splitting, which outperforms those of the state-of-the-art transition metal SACs. 相似文献
3.
Yanmin Hu Tingting Chao Yapeng Li Peigen Liu Tonghui Zhao Ge Yu Cai Chen Xiao Liang Huile Jin Shuwen Niu Wei Chen Dingsheng Wang Yadong Li 《Angewandte Chemie (International ed. in English)》2023,62(35):e202308800
Water electrolysis for H2 production is restricted by the sluggish oxygen evolution reaction (OER). Using the thermodynamically more favorable hydrazine oxidation reaction (HzOR) to replace OER has attracted ever-growing attention. Herein, we report a twisted NiCoP nanowire array immobilized with Ru single atoms (Ru1−NiCoP) as superior bifunctional electrocatalyst toward both HzOR and hydrogen evolution reaction (HER), realizing an ultralow working potential of −60 mV and overpotential of 32 mV for a current density of 10 mA cm−2, respectively. Inspiringly, two-electrode electrolyzer based on overall hydrazine splitting (OHzS) demonstrates outstanding activity with a record-high current density of 522 mA cm−2 at cell voltage of 0.3 V. DFT calculations elucidate the cooperative Ni(Co)−Ru−P sites in Ru1−NiCoP optimize H* adsorption, and enhance adsorption of *N2H2 to significantly lower the energy barrier for hydrazine dehydrogenation. Moreover, a self-powered H2 production system utilizing OHzS device driven by direct hydrazine fuel cell (DHzFC) achieve a satisfactory rate of 24.0 mol h−1 m−2. 相似文献
4.
Hongbo Yu Lixia Wang Huatong Li Zuyang Luo Dr. Tayirjan Taylor Isimjan Prof. Dr. Xiulin Yang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(60):e202201784
Metal-organic frameworks (MOFs) have been considered as potential oxygen evolution reaction (OER) electrocatalysts owning to their ultra-thin structure, adjustable composition, high surface area, and high porosity. Here, we designed and fabricated a vanadium-doped nickel organic framework (V1−x−NixMOF) system by using a facile two-step solvothermal method on nickel foam (NF). The doping of vanadium remarkably elevates the OER activity of V1−x−NixMOF, thus demonstrating better performance than the corresponding single metallic Ni-MOF, NiV-MOF and RuO2 catalysts at high current density (>400 mA cm−2). V0.09−Ni0.91MOF/NF provides a low overpotential of 235 mV and a small Tafel slope of 30.3 mV dec−1 at a current density of 10 mA cm−2. More importantly, a water-splitting device assembled with Pt/C/NF and V0.09−Ni0.91MOF/NF as cathode and anode yielded a cell voltage of 1.96 V@1000 mA cm−2, thereby outperforming the-state-of-the-art RuO2(+)||Pt/C(−). Our work sheds new insight on preparing stable, efficient OER electrocatalysts and a promising method for designing various MOF-based materials. 相似文献
5.
Dr. Ligang Wang Dr. Hui Su Zhuang Zhang Junjie Xin Hai Liu Dr. Xiaoge Wang Dr. Chenyu Yang Xiao Liang Dr. Shunwu Wang Dr. Huan Liu Yanfei Yin Taiyan Zhang Prof. Yang Tian Dr. Yaping Li Prof. Qinghua Liu Prof. Xiaoming Sun Prof. Junliang Sun Prof. Dingsheng Wang Prof. Yadong Li 《Angewandte Chemie (International ed. in English)》2023,62(49):e202314185
Developing cost-effective and sustainable acidic water oxidation catalysts requires significant advances in material design and in-depth mechanism understanding for proton exchange membrane water electrolysis. Herein, we developed a single atom regulatory strategy to construct Co−Co dinuclear active sites (DASs) catalysts that atomically dispersed zirconium doped Co9S8/Co3O4 heterostructure. The X-ray absorption fine structure elucidated the incorporation of Zr greatly facilitated the generation of Co−Co DASs layer with stretching of cobalt oxygen bond and S−Co−O heterogeneous grain boundaries interfaces, engineering attractive activity of significantly reduced overpotential of 75 mV at 10 mA cm−2, a breakthrough of 500 mA cm−2 high current density, and water splitting stability of 500 hours in acid, making it one of the best-performing acid-stable OER non-noble metal materials. The optimized catalyst with interatomic Co−Co distance (ca. 2.80 Å) followed oxo-oxo coupling mechanism that involved obvious oxygen bridges on dinuclear Co sites (1,090 cm−1), confirmed by in situ SR-FTIR, XAFS and theoretical simulations. Furthermore, a major breakthrough of 120,000 mA g−1 high mass current density using the first reported noble metal-free cobalt anode catalyst of Co−Co DASs/ZCC in PEM-WE at 2.14 V was recorded. 相似文献
6.
Yanling Qiu Zhiqiang Liu Qian Yang Xinyue Zhang Prof. Jingquan Liu Mengyao Liu Tianyi Bi Prof. Xuqiang Ji 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(51):e202200683
Combining the self-sacrifice of a highly crystalline substance to design a multistep chain reaction towards ultrathin active-layer construction for high-performance water splitting with atmospheric-temperature conditions and an environmentally benign aqueous environment is extremely intriguing and full of challenges. Here, taking cobalt carbonate hydroxides (CCHs) as the initial crystalline material, we choose the Lewis acid metal salt of Fe(NO3)3 to induce an aqueous-phase chain reaction generating free CO32− ions with subsequent instant FeCO3 hydrolysis. The resultant ultrathin (∼5 nm) amorphous Fe-based hydroxide layer on CCH results in considerable activity in catalyzing the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), yielding 10/50 mA ⋅ cm−2 at overpotentials of 230/266.5 mV for OER and 72.5/197.5 mV for HER. The catalysts can operate constantly in 1.0 M KOH over 48 and 45 h for the OER and HER, respectively. For bifunctional catalysis for alkaline electrolyzer assembly, a cell voltage as low as 1.53 V was necessary to yield 10 mA cm−2 (1.7 V at 50 mA cm−2). This work rationally builds high-efficiency electrochemical bifunctional water-splitting catalysts and offers a trial in establishing a controllable nanolevel ultrathin lattice disorder layer through an atmospheric-temperature chemical route. 相似文献
7.
Haitao Yuan Yanzhi Wang Dr. Chenxi Yang Dr. Zuozhong Liang Dr. Mingxing Chen Prof. Wei Zhang Prof. Haoquan Zheng Prof. Rui Cao 《Chemphyschem》2019,20(22):2964-2967
Hierarchical hollow nanocubes based on ultra-thin CoFe-layered double hydroxide (CoFe−LDH) nanosheets have been prepared. The obtained CoFe−LDH hollow nanocubes could effectively catalyze water oxidation at a low overpotential of 270 mV @ 10 mA cm−2, low Tafel slope of 58.3 mV dec−1 and show a long-term stability in alkali. 相似文献
8.
Shuo Li Yunxia Liu Kun Feng Chengyu Li Jiabin Xu Cheng Lu Prof. Haiping Lin Yong Feng Prof. Ding Ma Prof. Jun Zhong 《Angewandte Chemie (International ed. in English)》2023,62(39):e202308670
Electrochemical water splitting is a promising approach for producing sustainable and clean hydrogen. Typically, high valence state sites are favorable for oxidation evolution reaction (OER), while low valence states can facilitate hydrogen evolution reaction (HER). However, here we proposed a high valence state of Co3+ in Ni9.5Co0.5−S−FeOx hybrid as the favorable center for efficient and stable HER, while structural analogues with low chemical states showed much worse performance. As a result, the Ni9.5Co0.5−S−FeOx catalyst could drive alkaline HER with an ultra-low overpotential of 22 mV for 10 mA cm−2, and 175 mV for 1000 mA cm−2 at the industrial temperature of 60 °C, with an excellent stability over 300 h. Moreover, this material could work for both OER and HER, with a low cell voltage being 1.730 V to achieve 1000 mA cm−2 for overall water splitting at 60 °C. X-ray absorption spectroscopy (XAS) clearly identified the high valence Co3+ sites, while in situ XAS during HER and theoretical calculations revealed the favorable electron capture at Co3+ and suitable H adsorption/desorption energy around Co3+, which could accelerate the HER. The understanding of high valence states to drive reductive reactions may pave the way for the rational design of energy-related catalysts. 相似文献
9.
Tianyu Zhang Xu Han Hongbin Yang Prof. Aijuan Han Enyuan Hu Prof. Yaping Li Prof. Xiao-qing Yang Prof. Lei Wang Prof. Junfeng Liu Prof. Bin Liu 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(29):12153-12159
Single-atom catalysts (SACs) show great promise for electrochemical CO2 reduction reaction (CRR), but the low density of active sites and the poor electrical conduction and mass transport of the single-atom electrode greatly limit their performance. Herein, we prepared a nickel single-atom electrode consisting of isolated, high-density and low-valent nickel(I) sites anchored on a self-standing N-doped carbon nanotube array with nickel–copper alloy encapsulation on a carbon-fiber paper. The combination of single-atom nickel(I) sites and self-standing array structure gives rise to an excellent electrocatalytic CO2 reduction performance. The introduction of copper tunes the d-band electron configuration and enhances the adsorption of hydrogen, which impedes the hydrogen evolution reaction. The single-nickel-atom electrode exhibits a specific current density of −32.87 mA cm−2 and turnover frequency of 1962 h−1 at a mild overpotential of 620 mV for CO formation with 97 % Faradic efficiency. 相似文献
10.
Da-Huan Li Xiao-Yue Zhang Jiang-Quan Lv Ping-Wei Cai Yan-Qiong Sun Prof. Dr. Cai Sun Prof. Dr. Shou-Tian Zheng 《Angewandte Chemie (International ed. in English)》2023,62(46):e202312706
Inspired by the metal-oxo cluster structural feature and charge separation behaviour of the oxygen evolving center (OEC) in photosystem II (PS-II) under photoirradiation, a new crystalline photochromic polyoxomolybdate, MV2[β-Mo8O26] ( 1 , MV=methyl viologen cation), is designed as a biomimetic oxygen evolution reaction (OER) catalyst in neutral electrolytes. After photoinduced electron transfer (PIET) with colour change from colourless to grey, it remains in an ultra-stable charge-separated state over a year under ambient conditions. The observed overpotential at 10 mA ⋅ cm−2 and Tafel slope decrease by 49 mV and 62.8 mV ⋅ dec−1 after coloration, respectively. The outstanding OER performance of the coloured state in neutral electrolytes even outperforms the commercial RuO2 benchmark. Experimental and theoretical studies show that oxygen holes within polyanions after irradiation serve as sites for enhancing direct O−O coupling, thus effectively promoting OER. This is the first successful application of electron-transfer photochromism to realize OER activity gain. 相似文献
11.
Cheng Wang Prof. Limin Qi 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(39):17372-17377
The development of transition-metal-oxides (TMOs)-based bifunctional catalysts toward efficient overall water splitting through delicate control of composition and structure is a challenging task. Herein, the rational design and controllable fabrication of unique heterostructured inter-doped ruthenium–cobalt oxide [(Ru–Co)Ox] hollow nanosheet arrays on carbon cloth is reported. Benefiting from the desirable compositional and structural advantages of more exposed active sites, optimized electronic structure, and interfacial synergy effect, the (Ru–Co)Ox nanoarrays exhibited outstanding performance as a bifunctional catalyst. Particularly, the catalyst showed a remarkable hydrogen evolution reaction (HER) activity with an overpotential of 44.1 mV at 10 mA cm−2 and a small Tafel slope of 23.5 mV dec−1, as well as an excellent oxygen evolution reaction (OER) activity with an overpotential of 171.2 mV at 10 mA cm−2. As a result, a very low cell voltage of 1.488 V was needed at 10 mA cm−2 for alkaline overall water splitting. 相似文献
12.
Dr. Yongxiao Tuo Dr. Wanli Liu Dr. Chen Chen Dr. Qing Lu Prof. Yan Zhou Prof. Jun Zhang 《化学:亚洲杂志》2021,16(17):2511-2519
Electrocatalysts play a pivotal role in accelerating the sluggish electrochemical water splitting reaction. Herein, a Ru−Co oxides and carbon nitrides hybrid (RuCoOx/NC) electrocatalyst was constructed by employing ZIF-9 to disperse Ru precursor and deliberately regulating the calcination temperature. The moderate calcination temperature results in the RuCoOx nanocomposites with small particle size and low crystallinity as well as the co-existence of multi-valence metal compounds, thus boosting the amount and species of active sites. Moreover, the strong interactions between Co and Ru species induce the electron transfer from Co to Ru, thus enhancing the adsorption of anion intermediates on the electron-deficient Co species and the proton capturing capacity of electron-sufficient Ru species. As a result, the optimized RuCoOx/NC-350 catalyst behaved good electrocatalytic activities with 73 and 210 mV overpotential to achieve 10 mA cm−2 for HER and OER, respectively. Remarkably, it showed good durability by holding at 100 mA cm−2 for 100 h in HER and 50 mA cm−2 for 24 h in OER with small activity decline. This study may shed new light on the rational construction of highly efficient Ru-based catalysts for electrochemical water splitting. 相似文献
13.
Dr. Weijin Li Song Xue Sebastian Watzele Shujin Hou Johannes Fichtner A. Lisa Semrau Prof. Liujiang Zhou Dr. Alexander Welle Prof. Aliaksandr S. Bandarenka Prof. Roland A. Fischer 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(14):5886-5892
Metal–organic frameworks (MOFs) and their derivatives are considered as promising catalysts for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), which are important for many energy provision technologies, such as electrolyzers, fuel cells and some types of advanced batteries. In this work, a “strain modulation” approach has been applied through the use of surface-mounted NiFe-MOFs in order to design an advanced bifunctional ORR/OER electrocatalyst. The material exhibits an excellent OER activity in alkaline media, reaching an industrially relevant current density of 200 mA cm−2 at an overpotential of only ≈210 mV. It demonstrates operational long-term stability even at a high current density of 500 mA cm−2 and exhibits the so far narrowest “overpotential window” ΔEORR-OER of 0.69 V in 0.1 m KOH with a mass loading being two orders of magnitude lower than that of benchmark electrocatalysts. 相似文献
14.
Prof. Yao Wang Jiao Wu Shuaihao Tang Jiarui Yang Dr. Chenliang Ye Juan Chen Prof. Yongpeng Lei Prof. Dingsheng Wang 《Angewandte Chemie (International ed. in English)》2023,62(15):e202219191
Herein, we successfully construct bifunctional electrocatalysts by synthesizing atomically dispersed Fe−Se atom pairs supported on N-doped carbon (Fe−Se/NC). The obtained Fe−Se/NC shows a noteworthy bifunctional oxygen catalytic performance with a low potential difference of 0.698 V, far superior to that of reported Fe-based single-atom catalysts. The theoretical calculations reveal that p-d orbital hybridization around the Fe−Se atom pairs leads to remarkably asymmetrical polarized charge distributions. Fe−Se/NC based solid-state rechargeable Zn-air batteries (ZABs−Fe−Se/NC) present stable charge/discharge of 200 h (1090 cycles) at 20 mA cm−2 at 25 °C, which is 6.9 times of ZABs−Pt/C+Ir/C. At extremely low temperature of −40 °C, ZABs−Fe−Se/NC displays an ultra-robust cycling performance of 741 h (4041 cycles) at 1 mA cm−2, which is about 11.7 times of ZABs−Pt/C+Ir/C. More importantly, ZABs−Fe−Se/NC could be operated for 133 h (725 cycles) even at 5 mA cm−2 at −40 °C. 相似文献
15.
Kun Liu Zhuoya Zhu Mengqi Jiang Liangcheng Li Linfei Ding Dr. Meng Li Prof. Dongmei Sun Prof. Gaixiu Yang Prof. Gengtao Fu Prof. Yawen Tang 《Chemistry (Weinheim an der Bergstrasse, Germany)》2022,28(32):e202200664
An dual electronic and architectural engineering strategy is a good way to rationally design earth-abundant and highly efficient electrocatalysts of the oxygen evolution reaction (OER) for sustainable hydrogen-based energy devices. Here, a Ce-doped Co9S8 core–shell nanoneedle array (Ce−Co9S8@CC) supported on a carbon cloth has been designed and developed to accelerate the sluggish kinetics of the OER. Profiting from valance alternative Ce doping, a fine core–shell structure and vertically aligned nanoneedle arrayed architecture, Ce−Co9S8@CC integrates modulated electronic structure, highly exposed active sites, and multidimensional mass diffusion channels; together, these afford a favorable catalyzed OER. Ce−Co9S8@CC exhibits remarkable performance in the OER in an alkaline medium, where the overpotential requires only 242 mV to deliver a current density of 10 mA cm−2 for the OER; this is 70 mV superior to that of Ce-free Co9S8 catalyst and other counterparts. Good stability and impressive selectivity (nearly 100 % Faradic efficiency) are also demonstrated. When integrated into a two-electrode OER//HER electrolyzer, the as-prepared Ce−Co9S8@CC displays a low operation potential of 1.54 V at 10 mA cm−2 and long-term stability, thus demonstrating great potential for economical water electrolysis. 相似文献
16.
Dr. Dong Cao Dr. Zhirong Zhang Yahui Cui Runhao Zhang Prof. Lipeng Zhang Prof. Jie Zeng Prof. Daojian Cheng 《Angewandte Chemie (International ed. in English)》2023,62(9):e202214259
The construction of highly active, durable, and cost-effective catalysts is urgently needed for green hydrogen production. Herein, catalysts consisting of high-density Pt (24 atoms nm−2) and Ir (32 atoms nm−2) single atoms anchored on Co(OH)2 were constructed by a facile one-step approach. Remarkably, Pt1/Co(OH)2 and Ir1/Co(OH)2 only required 4 and 178 mV at 10 mA cm−2 for hydrogen evolution reaction and oxygen evolution reaction, respectively. Moreover, the assembled Pt1/Co(OH)2//Ir1/Co(OH)2 system showed mass activity of 4.9 A mgnoble metal−1 at 2.0 V in an alkaline water electrolyzer, which is 316.1 times higher than that of Pt/C//IrO2. Mechanistic studies revealed that reconstructed Ir−O6 single atoms and remodeled Pt triple-atom sites enhanced the occupancy of Ir−O bonding orbitals and improved the occupation of Pt−H antibonding orbital, respectively, contributing to the formation of the O−O bond and the desorption of hydrogen. This one-step approach was also generalized to fabricate other 20 single-atom catalysts. 相似文献
17.
Gangya Wei Dr. Yunxiang Li Dr. Xupo Liu Jinrui Huang Mengran Liu Dr. Deyan Luan Prof. Shuyan Gao Prof. Xiong Wen Lou 《Angewandte Chemie (International ed. in English)》2023,62(47):e202313914
Precise manipulation of the coordination environment of single-atom catalysts (SACs), particularly the simultaneous engineering of multiple coordination shells, is crucial to maximize their catalytic performance but remains challenging. Herein, we present a general two-step strategy to fabricate a series of hollow carbon-based SACs featuring asymmetric Zn−N2O2 moieties simultaneously modulated with S atoms in higher coordination shells of Zn centers (n≥2; designated as Zn−N2O2−S). Systematic analyses demonstrate that the synergetic effects between the N2O2 species in the first coordination shell and the S atoms in higher coordination shells lead to robust discrete Zn sites with the optimal electronic structure for selective O2 reduction to H2O2. Remarkably, the Zn−N2O2 moiety with S atoms in the second coordination shell possesses a nearly ideal Gibbs free energy for the key OOH* intermediate, which favors the formation and desorption of OOH* on Zn sites for H2O2 generation. Consequently, the Zn−N2O2−S SAC exhibits impressive electrochemical H2O2 production performance with high selectivity of 96 %. Even at a high current density of 80 mA cm−2 in the flow cell, it shows a high H2O2 production rate of 6.924 mol gcat−1 h−1 with an average Faradaic efficiency of 93.1 %, and excellent durability over 65 h. 相似文献
18.
Rui Liu Mingzi Sun Xiangjian Liu Zunhang Lv Xinyu Yu Jinming Wang Yarong Liu Liuhua Li Prof. Dr. Xiao Feng Prof. Dr. Wenxiu Yang Prof. Dr. Bolong Huang Prof. Dr. Bo Wang 《Angewandte Chemie (International ed. in English)》2023,62(46):e202312644
Developing highly efficient and stable hydrogen production catalysts for electrochemical water splitting (EWS) at industrial current densities remains a great challenge. Herein, we proposed a heterostructure-induced-strategy to optimize the metal-support interaction (MSI) and the EWS activity of Ru-Ni3N/NiO. Density functional theory (DFT) calculations firstly predicted that the Ni3N/NiO-heterostructures can improve the structural stability, electronic distributions, and orbital coupling of Ru-Ni3N/NiO compared to Ru-Ni3N and Ru-NiO, which accordingly decreases energy barriers and increases the electroactivity for EWS. As a proof-of-concept, the Ru-Ni3N/NiO catalyst with a 2D Ni3N/NiO-heterostructures nanosheet array, uniformly dispersed Ru nanoparticles, and strong MSI, was successfully constructed in the experiment, which exhibited excellent HER and OER activity with overpotentials of 190 mV and 385 mV at 1000 mA cm−2, respectively. Furthermore, the Ru-Ni3N/NiO-based EWS device can realize an industrial current density (1000 mA cm−2) at 1.74 V and 1.80 V under alkaline pure water and seawater conditions, respectively. Additionally, it also achieves a high durability of 1000 h (@ 500 mA cm−2) in alkaline pure water. 相似文献
19.
Xiaofang Bai Xiuping Zhang Yujiao Sun Mingcheng Huang Prof. Dr. Jiantao Fan Prof. Dr. Shaoyi Xu Prof. Dr. Hui Li 《Angewandte Chemie (International ed. in English)》2023,62(38):e202308704
To date, only a few noble metal oxides exhibit the required efficiency and stability as oxygen evolution reaction (OER) catalysts under the acidic, high-voltage conditions that exist during proton exchange membrane water electrolysis (PEMWE). The high cost and scarcity of these catalysts hinder the large-scale application of PEMWE. Here, we report a novel OER electrocatalyst for OER comprised of uniformly dispersed Ru clusters confined on boron carbon nitride (BCN) support. Compared to RuO2, our BCN-supported catalyst shows enhanced charge transfer. It displays a low overpotential of 164 mV at a current density of 10 mA cm−2, suggesting its excellent OER catalytic activity. This catalyst was able to operate continuously for over 12 h under acidic conditions, whereas RuO2 without any support fails in 1 h. Density functional theory (DFT) calculations confirm that the interaction between the N on BCN support and Ru clusters changes the adsorption capacity and reduces the OER energy barrier, which increases the electrocatalytic activity of Ru. 相似文献
20.
Dr. Sheng Yang Guangbo Chen Dr. Antonio Gaetano Ricciardulli Dr. Panpan Zhang Dr. Zhen Zhang Huanhuan Shi Ji Ma Dr. Jian Zhang Prof. Paul W. M. Blom Prof. Xinliang Feng 《Angewandte Chemie (Weinheim an der Bergstrasse, Germany)》2020,132(1):473-478
Transition-metal phosphides (TMPs) have emerged as a fascinating class of narrow-gap semiconductors and electrocatalysts. However, they are intrinsic nonlayered materials that cannot be delaminated into two-dimensional (2D) sheets. Here, we demonstrate a general bottom-up topochemical strategy to synthesize a series of 2D TMPs (e.g. Co2P, Ni12P5, and CoxFe2−xP) by using phosphorene sheets as the phosphorus precursors and 2D templates. Notably, 2D Co2P is a p-type semiconductor, with a hole mobility of 20.8 cm2 V−1 s−1 at 300 K in field-effect transistors. It also behaves as a promising electrocatalyst for the oxygen evolution reaction (OER), thanks to the charge-transport modulation and improved surface exposure. In particular, iron-doped Co2P (i.e. Co1.5Fe0.5P) delivers a low overpotential of only 278 mV at a current density of 10 mA cm−2 that outperforms the commercial Ir/C benchmark (304 mV). 相似文献