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Science China-Chemistry · 2022 ·Vol. 65 ·期 9 ·1829-1837 · IF 10.138

Amorphous/2H-MoS2 nanoflowers with P doping and S vacancies to achieve efficient pH-universal hydrogen evolution at high current density

Shi Yue,Zhang Dan,Miao Hongfu,Wu Xueke,Wang Zuochao,Zhan Tianrong,Lai Jianping,Wang Lei

Molybdenum disulfide (MoS 2 ) has become a competitive candidate for efficient and economical hydrogen evolution reaction (HER). Compared with 1T-MoS 2 , 2H-MoS 2 possesses exceptional thermodynamic stability but still suffers from low active site density, poor conductivity, and weak hydrogen bonding in the wide pH range. Herein, 2H-MoS 2 nanoflowers with phosphorus doping, sulfur vacancies and crystalline-amorphous heterojunction were synthesized via phosphorus-assisted rapid calcination method. Benefiting from the cooperative interaction of multiple strategies, the prepared 2H-MoS 2 nanoflowers firstly achieve efficient pH-universal HER at high current densities. Experimental results show that in alkaline, acidic, and neutral media, MoS 2 -P2 requires only 332, 302, and 417 mV to drive the current density of 500 mA cm −2 and obtains 932, 1100, and 472 mA cm −2 at the potential of −0.4 V vs. RHE, respectively. Moreover, MoS 2 -P2 shows excellent stability of low and high current density in the full pH range.

研究领域: 材料科学 · 电化学
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JOURNAL OF POWER SOURCES · 2025 · IF 7.9

Hydrophilicity and electronic structure modulation of Pb-doped RuO2 for pH-universal oxygen evolution catalysis

Xiaojing Dong,Jintao Wang,Yue Hao,Yiqiang Sun,Xu Zhang,Bo Xu,Cuncheng Li

Exploring oxygen evolution reaction (OER) electrocatalysts over a universal pH range to simultaneously achieve enhanced activity, improved stability and reduced cost is a rewarding yet challenging endeavor. Considering the hydrophilicity and electronegativity disparity between Pb and Ru, herein, a Pb doped RuO 2 catalyst and its application as electrocatalyst for OER under universal pH conditions are studied. Due to the modified hydrophilicity and electronic structure, the Pb 0.1 Ru 0.9 O 2 only requires an overpotential of 207 mV to obtain a current density of 10 mA cm −2 in acidic environment, and overpotentials of 232 mV and 363 mV are required in alkaline and neutral environments, respectively. Moreover, extensive stability assessments conducted over a 24-h period reveal remarkable stability of the catalyst in diverse environments, encompassing acidic, alkaline, and neutral conditions. Additionally, the utilization of density functional theory (DFT) computations offers persuasive evidence that the inclusion of Pb within RuO 2 can significantly alter its electronic configuration, thereby promoting efficient electron transfer processes. This modulation of the electronic structure is crucial for enhancing the catalytic performance of the material. This research paves the way for innovative designs of highly efficient oxygen evolution reaction (OER) catalysts, featuring minimized use of precious metals, heightened catalytic prowess, and unparalleled stability across a broad pH range.

研究领域: 材料科学 · 电化学 · 催化
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ELECTROCHIMICA ACTA · 2018 · IF 5.116

Fe-doped Co9S8 nanosheets on carbon fiber cloth as pH-universal freestanding electrocatalysts for efficient hydrogen evolution

Kelong Ao,Dawei Li,Yixin Yao,Pengfei Lv,Yibing Cai,Qufu Wei

Heteroatom doping is a feasible approach to adjust catalytic performance of the HER catalysts. In this work, we report a design of Fe-doped Co 9 S 8 nanosheets grown on carbon cloth (Fe-Co 9 S 8 NSs/CC) as a hydrophilic 3D monolithic electrocatalyst for efficient hydrogen evolution under all pH. The water contact angle and electrochemical measurements proved that the resultant material was hydrophilic for its nano hierarchitectures and dopant Fe enhanced the catalytic capability of singular Co 9 S 8 . In 1.0 M KOH, the Fe-Co 9 S 8 NSs/CC possessed a relatively small Tafel slope (95.3 mV dec −1 ) and required the overpotential of 83 mV to achieve 10 mA cm −2 . To drive the same current density, the overpotentials were 65 and 192 mV in 0.5 M H 2 SO 4 and 1.0 M PBS, respectively. Meanwhile, it showed good cycle stability and durability over 20 h static test at alkaline and neutral condition. The flexible freestanding catalyst has great potential in practical applications.

CAS / MDL: 7440-06-4
研究领域: 材料科学 · 电化学 · 催化
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Journal of Materials Chemistry A · 2023 ·Vol. 11 ·期 28 ·15227-15236 · IF 11.9

Universal passive radiative cooling behavior of aerogels

Bingjie Ma,Bing Wu,Peiying Hu,Ling Liu,Jin Wang

Aerogels have recently received extensive attention owing to their excellent thermal insulation performance. Thus, they are widely used for thermal management in buildings, aerospace, pipelines, and transportation for energy saving and emission reduction. However, silica aerogels have been confirmed to possess passive radiative cooling (PRC) capacities, which may seriously retard their thermal insulation performance. Therefore, whether PRC behavior is a universal property of aerogels is an urgent problem that can determine the eventual thermal management property of aerogels. Thus, in this study, six types of aerogels with different chemical components and microstructures, including silica aerogel, boron nitride aerogel, reduced-graphene oxide aerogel, Kevlar aerogel, poly(p-phenylene-2,6-benzobisoxazole) aerogel, and polyimide aerogels, are synthesized, and their PRC and thermal management behaviors are investigated. Impressively, all the above-mentioned aerogels showed extensive PRC performance, with a sub-ambient cooling ranging from 6.6 to 11.1 °C at night, regardless of their chemical component or color, confirming the universal PRC behavior of various aerogels. The PRC also significantly affects the thermal insulation properties of the aerogels. The reasons for the PRC of aerogels have been discussed. The findings of this study can help to a comprehensive understanding of the thermal management behavior of aerogels and guide to a better way to use aerogels in the actual environment by considering their PRC.

研究领域: 材料科学 · 能源工程
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Journal of Materials Chemistry A · 2020 ·Vol. 8 ·期 11 ·5595-5600 · IF 11.301

Transition metal M (M = Co, Ni, and Fe) and boron co-modulation in Rh-based aerogels for highly efficient and pH-universal hydrogen evolution electrocatalysis

Kai Deng,Tianlun Ren,You Xu,Songliang Liu,Zechuan Dai,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang

Although recent studies on the hydrogen evolution reaction (HER) have achieved great progress, it remains a great challenge to fabricate highly efficient pH-universal HER electrocatalysts. In this work, we report the facile synthesis of a new class of Rh-based spongy aerogels co-incorporated with transition metal M (M = Co, Ni, and Fe) and boron atoms through a simple and versatile one-pot wet-chemical strategy. Benefiting from the synergetic effect of 3D network-shaped spongy architectures and the electronic interaction between various elements, the optimized RhCoB aerogels exhibit excellent catalytic activity, stability and durability toward the HER in a wide pH range. The successful synthesis of RhMB aerogels will provide guidelines for designing and synthesizing an unprecedented class of transition metal and/or non-metal atom doped metallic materials toward potential catalysis and energy applications.

研究领域: 材料科学 · 电催化
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Nano Energy · 2017 · IF 12.343

In-situ activation of self-supported 3D hierarchically porous Ni3S2 films grown on nanoporous copper as excellent pH-universal electrocatalysts for hydrogen evolution reaction

C. Yang,M.Y. Gao,Q.B. Zhang,J.R. Zeng,X.T. Li,A.P. Abbott

The exploitation of low-cost, stable, and highly active electrocatalysts based on earth-abundant metals for hydrogen evolution reaction (HER) is crucial for developing renewable energy techniques. In this work, we report a facile synthesis strategy for in-situ fabrication of 3D hierarchically porous Ni 3 S 2 films on a nanoporous copper substrate (Ni 3 S 2 @NPC) by unusual galvanic replacement reaction in the Ethaline-based deep eutectic solvent (DES) under a normal atmosphere. The self-supported nanoporous Ni 3 S 2 @NPC electrode is binder- free and exhibits good structural integrity with high conductivity. A mild evolution of bulk gas bubbles (H 2 -O 2 gas mixture) is proved to drive an in-situ structure rearrangement process of the Ni 3 S 2 @NPC and results in substantial increases in the HER activity. The activated Ni 3 S 2 @NPC (a-Ni 3 S 2 @NPC) electrode can serve as a highly efficient and stable electrocatalyst for the HER in water over a wide pH range. Significantly, it displays high-performance HER catalytic activity in acidic media with robust durability over 111   h and functions well under alkaline and neutral conditions. Such a superior catalytic performance of the a-Ni 3 S 2 @NPC is mainly due to the unique hierarchically nanoporous architectures and the synergetic effects in it caused by the restructuring NPC skeletons and active components. Our work offers a generic strategy for design and fabrication of many other self-supported transition metal sulfide and phosphide based HER electrocatalysts, and uncovers a new O 2 -induced electrochemical self-activation mechanism for improving the activity of catalysts.

研究领域: 材料科学 · 电化学 · 可再生能源
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Advanced Science · 2021 ·Vol. 8 ·期 22 ·2102207 · IF 16.806

Facile Atomic-Level Tuning of Reactive Metal–Support Interactions in the Pt QDs@ HF-Free MXene Heterostructure for Accelerating pH-Universal Hydrogen Evolution Reaction

Sin-Yi Pang,Weng-Fu Io,Jianhua Hao

Supported metallic nanoparticles render highly tunable physical and chemical properties to mixed-dimensionality materials in electrocatalysts. However, some supports are susceptible to being dissolved in acidic solution or are unstable in ambient air. The development of high-performance catalysts has been facing the major hurdles of the sluggish activity in alkaline solution and requesting high energy to stabilize the nanoparticles on their supports, challenging the pH-universality and the applicability of the supported metallic nanoparticles. Here, a one-step strategy is proposed to modulate the growth of Pt quantum dots (QDs) on HF-free MXene under atomic-level by a low-temperature metal–support interaction reaction. By controllable tailoring in the morphology and strain induced by terminations, Pt (111) QDs with a sub-nanoscale size of 1.15 nm are grown as 0D/1D heterostructure to overcome the restrictions of employing reduction gas and high annealing temperature. The catalyst exhibits a low overpotential of 33.3 mV for acidic solution, while 65.1 mV for alkaline solution at a specific current density of 10 mA cm −2 . This study not only paves a scalable pathway to developing cost-efficient catalysts in moderate conditions, but also demonstrates an effective surface modulation strategy for 0D/1D heterostructures.

CAS / MDL: 9002-89-5
研究领域: 材料科学 · 电催化 · 纳米技术
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ACS Catalysis · 2024 · IF 11.3

Amorphous Ruthenium–Selenium Nanoparticles as a pH-Universal Catalyst for Enhanced Hydrogen Evolution Reaction

Ting Zhu,Junnan Han,Teng Sun,Jingjie Zhao,Xiaodong Pi,Jun Xu,Kunji Chen

In order to broaden the applications of water splitting for hydrogen production, it is highly desired to develop an ideal catalyst, which can operate in a wide pH range. In this work, we proposed amorphous RuSex nanoparticles (NPs) with a highly disordered structure to introduce abundant surface defects, which contribute to the enhanced HER activity. The optimized RuSe1.5 NPs exhibited the pH-universal activity, which only require an overpotential of 24, 30, and 12 mV to reach a current density of 10 mA cm–2 in 0.5 M H2SO4 (pH = 0), 1 M PBS (pH = 7), and 1 M KOH (pH = 14), respectively. By capitalizing on the synergistic effect between Ru and Se, we have successfully achieved a balance in the strong adsorption of reaction intermediates on Ru sites and significantly improved the performance of HER. This work highlights the crucial role of understanding and harnessing the elemental synergies in the development of optimized HER catalysts and paves the way for the advancement of hydrogen production.

研究领域: 材料科学 · 催化化学 · 能源科学
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InfoMat · 2025 · IF 22.3

RuO2 sub-nanocluster decorated Co3O4 as efficient and pH-universal oxygen evolution electrocatalyst

Ziye Li,Yangfan Liu,Jiandong Hu,Wenhui Luo,Yang Wang,Zhao Xin,Yanlin Jia,Yong Pang,Hong Zhang,Zhi Liang Zhao,Yejun Li,Qi Wang

Developing cost-effective and highly efficient oxygen evolution reaction (OER) electrocatalysts that operate in both acidic and alkaline media is crucial for industrial electrocatalytic water splitting. However, achieving high performance under dual pH conditions remains a significant challenge. Herein, we report the synthesis of multi-sized RuO 2 sub-nanoclusters on Co 3 O 4 nanoarrays via a facile method, which demonstrates exceptional OER activity in both acidic and alkaline environments. The optimized catalyst exhibits remarkably low overpotentials of 165 mV in 0.5 M H 2 SO 4 and 223 mV in 1 M KOH at a current density of 10 mA cm −2 , respectively. Additionally, it exhibits outstanding stability, maintaining performance over a 10-h continuous operation, which is attributed to the robust structural stability of the dispersed RuO 2 sub-nanocluster morphology. Atomic-scale investigations reveal a layer-by-layer growth mechanism of Ru on the Co 3 O 4 substrate, transitioning from single atoms to monolayer clusters and ultimately to sub-nanoclusters as Ru loading increases. This growth mechanism provides a rational strategy for the precise design and synthesis of advanced cluster-based catalysts. Density functional theory (DFT) calculations further elucidate the strong oxide-support interactions between RuO 2 clusters and the Co 3 O 4 matrix, facilitating electron transfer from RuO 2 to Co 3 O 4 and generating an electron-deficient region. This electronic modulation enhances –OH adsorption and accelerates OER kinetics. These findings underscore the potential of metal sub-nanoclusters for designing highly efficient and durable electrocatalysts for water electrolysis.

研究领域: 电化学 · 催化材料 · 能源转换与存储
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CHEMICAL ENGINEERING JOURNAL · 2021 · IF 13.273

Transition metal and phosphorus co-doping induced lattice strain in mesoporous Rh-based nanospheres for pH-universal hydrogen evolution electrocatalysis

Qiqi Mao,Shiqian Jiao,Kaili Ren,Shengqi Wang,You Xu,Ziqiang Wang,Xiaonian Li,Liang Wang,Hongjing Wang

Rhodium (Rh) -based nanomaterials are promising alternatives to platinum (Pt) for the hydrogen evolution reaction (HER). However, the engineering and synthesis of Rh-based electrocatalysts to achieve Platinum-like HER performance under a comprehensive pH range still remains a challenge. In this work, we report an effective tactics to promote the HER performance of Rh mesoporous nanoparticles (Rh MNs) by co-doping of transition metal (e.g., Ni, Co, Fe) and phosphorus (P) elements. Such a metal-nonmetal co-doping could effectively regulate the electronic structure, increase the active sites, and induce lattice strain, which jointly contributes to a superior HER performance. With these merits, the optimized RhNiP mesoporous nanoparticles (RhNiP MNs) exhibited superior HER activity in a comprehensive pH scope, requiring overpotentials of only 15 mV, 36 mV and 44 mV in 0.5 M H 2 SO 4 , 1 M KOH and 1 M phosphate buffer solution (PBS), respectively, at the cathodic current density for 10 mA cm −2 .

研究领域: 材料科学 · 电催化
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Energy & Environmental Science · 2021 ·Vol. 14 ·期 12 ·6455-6463 · IF 38.532

A pH-universal ORR catalyst with single-atom iron sites derived from a double-layer MOF for superior flexible quasi-solid-state rechargeable Zn–air batteries

Meiqi Zhao,Haoran Liu,Hongwei Zhang,Wen Chen,Hanqin Sun,Zhenhua Wang,Biao Zhang,Lin Song,Yong Yang,Chao Ma,Yunhu Han,Wei Huang

Developing a highly efficient, easy-to-fabricate and non-noble metal electrocatalyst is vital for the oxygen reduction reaction (ORR). Herein, we fabricate a single Fe site catalyst Fe1/d-CN by developing a double-layer MOF strategy. The Fe1/d-CN catalyst shows an excellent ORR activity in the pH-universal range, especially in alkaline electrolytes with a record-level half-wave potential of 0.950 V, exceeding those of almost all the reported non-noble electrocatalysts and the commercial Pt/C catalyst (0.863 V). Besides its exceptional ORR activity in alkaline electrolytes, it also exhibits comparable ORR activity to the commercial Pt/C catalyst in acidic and neutral electrolytes. We speculate that the sources of the excellent pH-universal ORR performance can be attributed to the regulation of the electronic structure of Fe centres and the excellent electron/proton transport capability that comes from the rich defects and hierarchical porous features of the Fe1/d-CN catalyst. More excitingly, the catalyst possesses remarkable durability, and exhibits a negligible decrease after 30k accelerated durability test (ADT) cycles in pH-universal media. The flexible quasi-solid-state alkaline rechargeable Zn–air batteries with the Fe1/d-CN catalyst as the cathode show superior performance such as a high OCV of 1.50 V and peak power density of 78.0 mW cm−2. Furthermore, the flexible quasi-solid-state neutral rechargeable Zn–air batteries also exhibited remarkable performance.

研究领域: 材料科学 · 电化学 · 能源科学
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Journal of Physical Chemistry C · 2021 · IF 4.126

Engineering Efficient NiIrx/CNT Hybrid Nanostructures for pH-Universal Oxygen Evolution

Yuyan Qiao,Yanqiu Pan,Shiwen Du,Tingting Wu,Yucheng Cao,Guifa Long,Wenjun Fan,Fuxiang Zhang

Development of highly efficient and pH-universal oxygen evolution reaction (OER) electrocatalysts with reduced noble metal dosage while enhancing catalytic performance is essential for the commercial application of water electrolyzers. Here, we report the NiIrx/carbon nanotube (CNT) hybrid nanostructures in situ grown on carbon fiber paper (CFP) substrate for efficient OER in wide pH ranges. In 0.5 M H2SO4, the resulting NiIrx/CNT/CFP electrode only demands 196 mV overpotential to achieve 10 mA cm–2, which is significantly superior to those of the Ni/CNTs, Ir/CNTs, and NiIrx samples. Meanwhile, it also shows high performance in alkaline solution with a low overpotential of 220 mV at 10 mA cm–2. The in situ grown approach guarantees the intimate contact between the substrate and the catalyst, and the CNTs provide high conductivity and high exposed surface area for active sites. Furthermore, the introduction of Ni triggered electronic coupling between Ir and Ni that regulates the adsorption energy for the OER intermediates, as indicated by density functional theory calculations. This work demonstrates the cooperative effect not only between the noble metals and the support but also between noble metals and the non-noble metals for the OER.

CAS / MDL: 13478-00-7
研究领域: 材料科学 · 电化学 · 催化科学
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