ACS Applied Materials & Interfaces
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2015
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IF 6.723
Liang-Liang Feng,Guo-Dong Li,Yipu Liu,Yuanyuan Wu,Hui Chen,Yun Wang,Yong-Cun Zou,Dejun Wang,Xiaoxin Zou
Splitting water to produce hydrogen requires the development of non-noble-metal catalysts that are able to make this reaction feasible and energy efficient. Herein, we show that cobalt pentlandite (Co9S8) nanoparticles can serve as an electrochemically active, noble-metal-free material toward hydrogen evolution reaction, and they work stably in neutral solution (pH 7) but not in acidic (pH 0) and basic (pH 14) media. We, therefore, further present a carbon-armoring strategy to increase the durability and activity of Co9S8 over a wider pH range. In particular, carbon-armored Co9S8 nanoparticles (Co9S8@C) are prepared by direct thermal treatment of a mixture of cobalt nitrate and trithiocyanuric acid at 700 °C in N2 atmosphere. Trithiocyanuric acid functions as both sulfur and carbon sources in the reaction system. The resulting Co9S8@C material operates well with high activity over a broad pH range, from pH 0 to 14, and gives nearly 100% Faradaic yield during hydrogen evolution reaction under acidic (pH 0), neutral (pH 7), and basic (pH 14) media. To the best of our knowledge, this is the first time that a transition-metal chalcogenide material is shown to have all-pH efficient and durable electrocatalytic activity. Identifying Co9S8 as the catalytically active phase and developing carbon-armoring as the improvement strategy are anticipated to give a fresh impetus to rational design of high-performance noble-metal-free water splitting catalysts.
研究领域:
材料科学
·
化学
✓ 已验证
DOI
高影响因子
JOURNAL OF SOLID STATE CHEMISTRY
·
2024
·
IF 3.2
Yuning Wang,Yang Chen,Yongjian Xu,Yatao Yan,Ming Chen,Mengting Shao,Qianhui Wu,Fang Guo,Jianhua Hou
The development of cheap, efficient and stable hydrogen-producing catalysts is the current research focus, especially the catalysts that can work stably in the whole pH range. In this work, a myrica rubra-like structure of P–Co 1-x S/C was synthesized by hydrothermal reaction, sulfurization and phosphorization using spherical flower-like cobalt glycerate (CoG) as precursor. The design of this multilevel structure of P–Co 1-x S/C effectively increases the specific surface area. The doping phosphorus and the protection of carbon layer greatly improve catalytic performance and enhance the stability of Co 1-x S in the hydrogen evolution reaction (HER) at full pH range. When the current density is 10 mA cm −2 , the HER overpotentials of P–Co 1-x S/C in acidic, alkaline and neutral solutions are 86, 93 and 167 mV, and respectively. The Tafel slopes of P–Co 1-x S/C in acidic, alkaline and neutral solutions are 82, 100 and 103 mV dec −1 , respectively. In addition, the electrocatalyst also displays excellent electrochemical long-term stability. After 2000 cycles or 20 h long-term testing, its catalytic activity remains stable without obvious decrease at full pH range.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Yong Jiang,Yini Mao,Yimin Jiang,Hao Liu,Wei Shen,Ming Li,Rongxing He
Developing bifunctional electrocatalysts with high activity and long-term stability over the whole pH range is still a great challenge. Herein, the unsupported RuIr alloys are reported as robust electrocatalysts for pH-universal overall water splitting. The as-synthesized Ru 0.5 Ir 0.5 alloy exhibits unexpected low overpotentials of 4, 28, 16 mV for hydrogen evolution reaction (HER) and 160, 176, 248 mV for oxygen evolution reaction (OER) at 10 mA cm −2 in 0.5 M H 2 SO 4 , 1.0 M KOH and 1.0 M PBS solutions, respectively. Especially, the Ru 0.5 Ir 0.5 ||Ru 0.5 Ir 0.5 cell only needs voltages of 1.44, 1.48 and 1.51 V in the three environments to reach the same current density for overall water splitting and can continuously operate for more than 400, 100 and 100 h. Comprehensive studies verify that the excellent electrocatalytic performance of Ru 0.5 Ir 0.5 originates from the uniform arrangement of Ru and Ir atoms in the alloy, which leads to the leaching of an appropriate amount of Ru atoms and thus produces a protective skeleton composed of high valence Ir (IV) to prevent further dissolution of Ru. In addition, the weak coupling between Ru and Ir makes electron transfer from Ir to adjacent Ru as active sites, resulting in optimal adsorption strength for key intermediates.
研究领域:
材料科学
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电化学
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF ELECTROANALYTICAL CHEMISTRY
·
2025
·
IF 4.1
Qianqian Song,Yang Chen,Yongjian Xu,Yatao Yan,Qianhui Wu,Fang Guo,Ming Chen,Guowang Diao
Hydrogen energy represents a form of green energy, and the electrolysis of water for hydrogen production is recognized as an efficient method. Current research is primarily focused on the development of catalysts that are both efficient and stable, particularly those capable of functioning consistently across the entire pH spectrum. In this work, Co 9 S 8 /NC co doped with N and P was successfully synthesized through a series of sulfurization, calcination, and phosphating operations using dual ligand Co-ZIF as the precursor. By coating a carbon layer and co doping with nitrogen and phosphorus, the catalytic performance and stability of hydrogen evolution reaction (HER) were significantly improved over the entire pH range. At a fixed current density of 10 mA cm −2 , the overpotential of HER was measured at voltages of 136, 96, and 194 mV in three different pH solutions. Furthermore, the electrocatalyst exhibits remarkable electrochemical stability over extended periods. After 20 h or 2000 cycles of testing, the catalytic activity did not show a significant decrease across the entire pH range, but rather exhibited a relatively sustained constant.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2023
·
IF 7.2
Peng Cui,Tongheng Wang,Xuhai Zhang,Chongyang Ba,Yangkun Wu,Kai Peng,Yuqiao Zeng,Jianqing Jiang
Though various active electrocatalysts for hydrogen evolution reaction (HER) have been reported, it remains a challenge to develop efficient non-noble HER catalysts with pH-independent catalytic activity and high stability. In this work, novel porous NiCoCuP was prepared by combining the dynamic hydrogen bubble templated deposition with a low-temperature phosphorization process. The three-dimensional hierarchical porous structure provided the NiCoCuP with both self-supporting ability and ideal channels for fast mass transportation. As a consequence, the NiCoCuP foam exhibited excellent HER catalytic activity and outstanding durability over the entire pH range.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2024
·
IF 9.4
Yao Tang,Chunyan Fan,Zehao Zang,Yahui Cheng,Lanlan Li,Xiaofei Yu,Xiaojing Yang,Zunming Lu,Xinghua Zhang,Hui Liu
Producing hydrogen through water electrolysis represents a clean and sustainable solution that is crucial in addressing the energy crisis. Nonetheless, the slow process of water electrolysis leads to large different kinetics for hydrogen evolution reaction (HER) under different pH solutions. Here, we designed surface modified metallic X-Cu catalysts (X = F, Cl, Br) with different non-metallic elements on nickel foam (NF) using an electrochemical deposition method, which realizes high performance for all-pH range. In 1.0 M KOH, 1.0 M phosphate-buffered saline (PBS), and 0.5 M H 2 SO 4 media, F-Cu catalyst reaches 10 mA cm −2 with overpotentials of 56 mV, 110 mV, and 197 mV, respectively. Theoretical calculations disclose that the surface modification of F atom leads to redistribution of electrons, causing an upward shift of Cu’s d-band center and enhanced adsorption ability for H 2 O and H intermediates (H*). This work offers novel perspectives for designing Cu-based catalysts with high HER performance, making them applicable across all-pH conditions.
研究领域:
材料科学
·
能源化学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of Energy Chemistry
·
2021
·
IF 9.676
Minmin Wang,Min Li,Yilin Zhao,Naiyou Shi,Hui Zhang,Yuxue Zhao,Yaru Zhang,Haoran Zhang,Wenhong Wang,Kaian Sun,Yuan Pan,Shoujie Liu,Houyu Zhu,Wenyue Guo,Yanpeng Li,Yunqi Liu,Chenguang Liu
The development of low-cost, efficient, and high atomic economy electrocatalysts for hydrogen evolution reaction (HER) in the entire pH range for sustainable hydrogen production is of great importance but still challenging. Herein, we synthesize a highly dispersed N-doped carbon frames (NCFs) anchored with Co single atoms (SAs) and Co nanoparticles (NPs) catalyst by a doping-adsorption-pyrolysis strategy for electrocatalytic hydrogen evolution. The Co SAs-Co NPs/NCFs catalyst exhibits an excellent HER activity with small overpotential, low Tafel slope, high turnover frequency as well as remarkable stability. It also exhibits a superior HER performance in the entire pH range. Combining with experimental and theoretical calculation, we find that Co SAs with Co-N 3 coordination structure and Co NPs have a strong interaction for promoting synergistic HER electrocatalytic process. The H 2 O molecule is easily activated and dissociated on Co NPs, while the generated H* is easily adsorbed on Co SAs for HER, which makes the Co SAs-Co NPs/NCFs catalyst exhibit more suitable H adsorption strength and more conducive to the activation and dissociation of H 2 O molecules. This work not only proposes a novel idea for constructing coupling catalyst with atomic-level precision, but also provides strong reference for the development of high-efficiency HER electrocatalysts for practical application.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
TRANSACTIONS OF TIANJIN UNIVERSITY
·
2025
·
IF 8.5
Sun Siyu,Zhang Feifei,Liu Wanlin,Zhang Rui,Yin Pengfei,Yang Jing,Dong Cunku,Nie Xinming,Liu Hui,Du Xiwen
The development of highly active and cost-effective catalysts for the full pH range of the hydrogen evolution reaction (HER) to meet the industrial application demands is an urgent challenge. In this work, the performance and structure–activity relationships of CuIr alloys prepared by the pulsed laser ablation in liquid technique as full pH range HER catalysts were investigated. Results indicated that Ir is doped into the Cu matrix as single atoms in CuIr-0.1, and CuIr-0.1 single-atom alloys (SAAs) exhibit superior HER performance and stability across the full pH range, with overpotentials of 135, 203, and 172 mV at the current density of 10 mA/cm 2 in acidic, neutral, and alkaline electrolytes, respectively. The enhanced performance of CuIr-0.1 SAAs can be attributed to the abundant active sites and accelerated reaction kinetics brought about by the electronic effects. This work successfully alloyed two immiscible metals to improve the catalytic performance, providing an avenue for the development of highly efficient and versatile HER catalysts for industrial applications.
研究领域:
材料科学
·
电化学
·
能源催化
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2019
·
IF 4.084
Qian Luo,Caili Xu,Qian Chen,Jie Wu,Yi Wang,Yun Zhang,Guangyin Fan
Pt-group metal phosphides are widely utilized as efficient electrocatalysts for hydrogen evolution reaction (HER), whereas most of the synthetic strategies are complicated, dangerous, and toxic with the use of large amount of nitrogen (N) and/or phosphorus (P) sources. Here, we report the synthesis of ruthenium phosphide nanoparticles (NPs) confined into N/P dual-doped carbon by pyrolyzing self-prepared ruthenium-organophosphine complex using 1,3,5-triaza-7-phosphadamantane (PTA) as the ligand and N/P sources. The achieved S–RuP 2 /NPC displayed excellent electrocatalytic activity (overpotentials of 19, 37, and 49 mV in alkaline, neutral, and acidic media, respectively, at 10 mA cm −2 ) toward HER at all pH ranges. The high performance of S–RuP 2 /NPC must be ascribed to the homogeneously distributed and P-rich RuP 2 NPs with the diameter of 3.29 nm on the NPC surface, which can considerably improve the atom utilization for HER. The present synthetic strategy not only avoids the use of additional N/P sources but also the generation of flammable and toxic PH 3 gas. This synthetic strategy can be extended to prepare other traditional metal phosphides for electrocatalytic applications.
研究领域:
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2025
·
IF 8.3
Conghan Zhang,Jiating Cheng,Fan Yang,Yang Sun,Xinyang Sun,Kexin Wei,Guang Ma,Junpu An,Meitong Zhao,Jiahui Liu,Yongfeng Li
Electrolytic water splitting using transition metal sulfide catalysts has garnered a lot of attention lately. Herein, a composite material consisting of Mo-doped Ni 3 S 2 nanoparticles supported on N-doped carbon layers with anchored Ni single atoms (Mo–Ni 3 S 2 /Ni–N–C) was synthesized using a two-step hydrothermal process. These features enable Mo–Ni 3 S 2 /Ni–N–C to achieve low overpotentials of 71, 58, and 89 mV for the hydrogen evolution reaction (HER) at 10 mA cm −2 in 1 M KOH, 0.5 M H 2 SO 4 , and 1 M PBS, respectively. After 20 h of durability testing, its current density retains over 95 % of the initial value across diverse pH electrolytes. Mo doping enhances structural stability, enabling wide pH applicability. Electron transfer from Ni 3 S 2 nanoparticles to Ni single atoms accelerates kinetics and boosts intrinsic activity, which improves HER performance. Theoretical calculations confirm that Ni single atoms possess ideal H∗ adsorption energy, which optimizes H∗ adsorption capability of Ni 3 S 2 . This work offers suggestions for creating excellent low-cost electrolytic water catalysts.
研究领域:
电化学
·
催化
·
材料科学
·
纳米技术
·
能量转换
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）