LANGMUIR
·
2026
·Vol. 42
·期 31
·22950-22957
·
IF 4.4
Chen Nannan,Yuan Qingle,Liu Qin,Zhang Chao,Wu Zhengcui,Bi Wentuan
Single-atom catalysts (SACs) hold great promise for the
electrochemical
reduction of CO 2 to CO; however, the high selectivity is
typically restricted within a narrow potential window, limiting their
practical implementation. In this study, Ni–N–C catalysts
were supported on ordered and disordered carbon nanofiber membranes
(denoted as o-NiNC and d-NiNC, respectively) via electrospinning to
elucidate the effect of nanofiber alignment on CO 2 reduction
activity. The results demonstrate that o-NiNC catalysts allow for
spatially uniform H + /CO 2 delivery and consumption,
thereby mitigating the selectivity variations arising from uneven
spatial distribution of reactants. As a result, the o-NiNC catalysts
achieve a CO Faradaic efficiency (FE) of 98.5% at −1.0 V and
maintain an FE above 90% across a broad potential range (−0.6
to −1.6 V). This work provides new insights into the rational
design of high-performance CO 2 reduction electrocatalysts
through geometric engineering.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2022
·
IF 7.139
Zi-Hao Zhang,Lin-Chang Liu,Chen-Xi Zhang,Hong-Lin Zhu,Yue-Qing Zheng
Alloy catalyst has been widely studied and used for hydrolytic dehydrogenation of ammonia borane (NH 3 BH 3 , AB) with excellent catalytic performance due to the synergistic effect of bimetal . Herein, a series of Rh 1-x Co x /Ni@Ni–N–C catalysts were prepared by an impregnation reduction method. The optimized Rh 0.75 Co 0.25 /Ni@Ni–N–C catalyst exhibited good catalytic performance with turnover frequency of 223.08 mol H2 mol cat −1 min −1 at 303 K, but decreased the catalytic performance compared with Rh/Ni@Ni–N–C. According to the XPS and Raman analysis, the RhCo alloy nanoparticles could be loaded at the defect position of Ni@Ni–N–C, and the Co nanoparticles occupied the intercalation between Rh and the defective site of the carrier, which could weaken the catalytic activity of AB hydrolysis. Based on the above research, we proposed the catalytic mechanism of the activation of the RhCo–H species. This work provides a new strategy for designing alloy-supported nano-catalysts.
✓ 已验证
产品关联
DOI
高影响因子
ChemSusChem
·
2023
·
IF 8.4
Jiaji Zhang,Gaobo Lin,Jie Zhu,Sifan Wang,Wenhua Zhou,Xiangzhou Lv,Bolong Li,Jianghao Wang,Xiuyang Lu,Jie Fu
Graphical We find that the N-doped Ni particles can enhance the adsorption of CO 2 and modulate the configuration of adsorbed CO on Ni-N-C sites. As a result, the optimal catalyst can efficiently convert CO 2 into CO with a faradaic efficiency of 96.7 % and a current density of 500 mA cm −2 in a strongly acidic electrolyte. Electro-chemically reducing CO 2 in a highly acidic medium is promising for addressing the issue of carbonate accumulation. However, the hydrogen evolution reaction (HER) typically dominates the acidic CO 2 reduction. Herein, we construct an efficient electro-catalyst for CO formation based on a core-shell structure, where nitrogen-doped Ni nanoparticles coexist with nitrogen-coordinated Ni single atoms. The optimal catalyst demonstrates a significantly improved CO faradaic efficiency (FE) of 96.7 % in the acidic electrolyte (pH=1) at an industrial-scale current density of 500 mA cm −2 . Notably, the optimal catalyst maintains a high FE of CO exceeding 90 % (current density=500 mA cm −2 ) in the electrolyte with a wide pH range from 0.67 to 14. In-situ spectroscopic characterization and density functional theory calculations show that the local electron density of Ni-N-C sites is enhanced by N-doped Ni particles, which facilitates the formation of *COOH intermediate and the adsorption of *CO. This study demonstrates the potential of a hybrid metal/Ni-N-C interface in boosting acidic CO 2 electro-reduction.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ADVANCED FUNCTIONAL MATERIALS
·
2025
·
IF 19
Mingdong Sun,Shibo Xi,Siyu Zhu,Yu Zhou,Changping Li,Biao Meng,Jiao Wei,Xiao Chi,Xiaojiang Yu,Yujie Cao,Yizhong Huang,Xiaoling Liu,Jun Wang
N-doped carbon-supported single-atom metal sites (Me−N−C) have emerged as promising candidates for electrochemical CO 2 reduction reaction (CO 2 RR) under industrial current densities. However, rationalizing their local coordination environment remains challenging. Herein, a feasible strategy is demonstrated for constructing robust Ni─N─C centers by designing a new family of single-crystalline ionic ZIF-8 materials with atomically defined ionic liquid (IL) cations inside the microchannels. The ─COOH tethered ionic ZIF-8 directed the formation of atomically dispersed Ni─N 4 sites with an elongated Ni─N bond of 1.94 Å. The resulting Ni─N─C catalyst effectively catalyzed the electrochemical CO 2 reduction to CO, delivering a partial current density of 679 mA cm −2 with a Faradic efficiency of 97% and achieving a maximum turnover frequency of 106197 h −1 . The extended Ni─N bond enables the slightly reduced valence state of the Ni site, optimizing the affinity toward CO 2 and intermediate, and thus lowering the energy barrier in the rate-determining * CO 2 → * COOH step.
✓ 已验证
DOI
高影响因子
ACS Applied Energy Materials
·
2021
·
IF 6.024
Lin-Chang Liu,Hong-Lin Zhu,Yue-Qing Zheng
Ammonia borane (NH3BH3, referred to as AB) hydrolytic dehydrogenation is regarded as a feasible strategy for hydrogen production owing to its high hydrogen content, pollution-free nature, and high stability. Metal nitrogen-doped carbon materials (M-N-C) are considered as an ideal candidate support of catalysts with AB hydrolytic dehydrogenation due to the advantages of low cost, large specific surface area, rich defective site, and good chemical stability. In this work, tubular Ni@Ni-N-C was successfully synthesized by high-temperature pyrolysis, and then, Rh nanoparticles were decorated on the support Ni@Ni-N-C by impregnation and reduction to prepare a series of Rh/Ni@Ni-N-C. The best catalytic performance of catalysts is obtained using Ni@Ni-N-C with an Rh loading of 0.74 wt %, showing a turnover frequency as high as 782.18 min–1 and an apparent activation energy (Ea) as low as 25.86 kJ mol–1, which could be attributed to the strong interaction between Rh and the defective site of the support.
✓ 已验证
产品关联
DOI
高影响因子
Green Chemical Engineering
·
2022
·
IF 0
Jianguo Liu,Jiangmin Sun,Thishana Singh,Shanshan Lin,Longlong Ma
Although precious transition metals such as palladium, platinum, and iridium are widely used in hydrogenation reactions, the earth-abundant transition metal-catalyzed highly selective semi-hydrogenation of terminal alkynes to terminal alkenes remains poorly developed and a challenge. Herein we demonstrate the excellent selective, cost-effective semi-hydrogenation of terminal alkynes via a novel graphene encapsulated Ni@N/C catalyst. The graphene layer encapsulated nano-catalyst Ni@N/C could significantly avoid metal leaching and improve the stability of the catalyst. The strong interaction of nitrogen with the Ni nanoparticles regulates the activity of Ni towards selective semi-hydrogenation of terminal alkynes. Substrates having un-functionalized as well as functionalized substituents, and substrates having sensitive functional groups (olefins, ketones) which pose a challenge to hydrogenate, were semi-hydrogenated with excellent conversion (up to 99%) and selectivity (up to 99%) under optimized reaction conditions.
✓ 已验证
DOI
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.
✓ 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）