Kuei-Hsien Chen

An innovative strategy has been developed to activate the basal planes in molybdenum disulfide (MoS2) to improve their electrocatalytic activity by controlling surface electron accumulation (SEA) through aging, annealing, and nitrogen-plasma treatments. The optimal hydrogen evolution reaction (HER) performance was obtained on the surface treated with nitrogen-plasma for 120 s. An overpotential of 0.20 V and a Tafel slope of 120 mV dec−1 were achieved for the optimized condition. The angle-resolved photoemission spectroscopy measurement confirmed the HER efficiency enhanced by the SEA conjugated with the sulfur vacancy active sites in the MoS2 basal planes. This study provides new insight into optimizing MoS2 catalysts for energy applications.

Achieving lithium-ion batteries with both excellent electrochemical performance and cycling stability is a top priority for their real-world applications. This work reports high-performance and stable Cu2ZnSnS4 (CZTS) anode materials encapsulated by nitrogen-doped carbon (CZTS@N-C) for advanced lithium-ion battery application. Ex-situ X-ray photoelectron spectroscopy and transmission electron microscopy revealed that the nitrogen-doped carbon network features a more conducive solid-electrolyte interphase that enables lower charge-transfer resistance and fast Li+ diffusion kinetics with negligible initial irreversible capacity loss. As a result, the CZTS@N-C electrode delivers a significantly enhanced capacity of 710 mAh g−1 with 73% capacity retention after 220 cycles at a current rate of 0.5 mA g−1 and superior rate performance compared to that of unmodified CZTS. Additionally, the study sheds light on the fast lithiation dynamics chemistry of CZTS@N-C through kinetics analysis, explored by in-situ Raman, ex-situ X-ray absorption, and in-situ electrochemical impedance. This study provides a new approach for fabricating high-performance, durable conductive polymer-encapsulated low-cost transition-metal-sulfide anode materials.

As a lead-free high-performance thermoelectric material, germanium telluride (GeTe) has recently been extensively studied for mid-temperature (500–800 K) applications. The carrier concentration and the thermal conductivity are reduced for vacancy-controlled GeTe compounds compared with pristine GeTe. We explored and optimized the Ge0.9−xSb0.1PxTe (x = 0.01–0.05) material's highest thermoelectric performance at elevated temperatures. Intrinsic Ge vacancy control and manipulation of Ge (+2) with Sb/P (+3) increased the charge contribution to power factor improvement to ∼42 µWcm−1 K−2 while minimizing the lattice thermal contribution to ∼0.4 W/mK. This resulted in an increase in thermoelectric performance of ∼2.4 @ 773 K for the Ge0.88Sb0.1P0.02Te sample. The inclusion of atomically disordered Sb/P ions considerably increases the scattering effects caused by the point defect, whereas stretched grain boundaries reveal the decreased lattice thermal contribution. The current work demonstrates the effectiveness of phosphorus as a co-dopant in increasing the average thermoelectric performance (ZTavg) value over the GeTe operating temperature range.

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A fine control of carriers in solids is the most essential thing while exploring any functionality. For a ternary skutterudite like CoSn1·5Te1.5−x, which has been recently recognized as a potential material for thermoelectric conversion, the dominant carrier could be either electrons or holes via chemically tuning the quaternary Sn2Te2 rings in the structure. Both theoretical calculation and different spectroscopic probes, such as X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) were employed to unveil the conduction type switching details. On the other hand, a Ni-for-Co substitution was applied to enhance electronic transport, and thereby the thermoelectric power factor. Thanks to the substantial cut-off of lattice thermal conductivity by the characteristic Sn2Te2 rings in the skutterudite structure, ultimately a 70-fold increase in the dimensionless figure-of-merit (zT) is achieved at 723 K with the nominal composition Co0·95Ni0·05Sn1·5Te1.5.

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Tin monosulfide (SnS) is a promising light-harvesting material for solar cell applications, owing to its potential for large-scale production, cost-effectiveness, eco-friendly source materials, and long-term stability. However, SnS crystallizes in an orthorhombic structure, which results in a highly anisotropic charge transport behavior. Tailoring the crystallographic orientation of the SnS absorber layer plays a critical role in the enhancement of the transfer of charge carriers and the power conversion efficiency (PCE). By controlling the substrate tilting angle and temperature ramp rate in vapor transport deposition, the crystal growth orientation was tuned to a preferred direction which significantly suppressed the unfavorable (040) crystallographic plane. Through the combination of these two approaches, the PCE could be increased from 0.11% to 2%. The effect of the tilting angle was numerically simulated to investigate its role in controlling the film uniformity and directing the film growth. In addition, the correlation between the texture coefficient of the (040) plane and the charge transport properties was determined by a combination of analytical methods such as device performance studies, electrochemical impedance spectroscopy, along with transient photovoltage, space-charge-limited current, and dark current measurements. These techniques were blended together to prove that the marked improvement in PCE can be ascribed to a reduced charge recombination (in both SnS bulk and interfaces) and an enhanced hole mobility.

Exploring an efficient platinum group metal (PGM) free electrocatalyst with superior activity and stability for hydrogen evolution reaction (HER) in a wide pH range is desirable for low-cost hydrogen production. Here, we report atomically dispersed cobalt on nitrogen and sulfur co-doped graphene (N-Co-S/G) for HER. Remarkably, the prepared N-Co-S/G electrocatalyst shows a small overpotential of 67.7 mV vs. reversible hydrogen electrode (RHE) at a current density of 10 mA cm−2 and exceptional durability over 100 h at 10 mA cm−2 under acidic conditions. Moreover, we found that the HER activity of N-Co-S/G is close to 20% Pt/C at all pH levels (0–14) and superior activity at high current density (>100 mA cm−2). Experimental and theoretical calculations reveal that the S atom in N-Co-S/G form Co-S bond, resulting new Co-N3S1 active site, which optimizes Gibbs free energy for hydrogen adsorption (∆GH*) close to zero, while water adsorption and dissociation enhanced by S modulation for neutral and basic media HER.

Thermoelectric (TE) devices used to convert waste heat directly into electricity are highly desirable for alleviating the prevailing energy crisis and global climate-change issues. Among the various TE materials available, metal oxides exhibit high thermal and chemical stabilities in air, and are hence, preferred for use in many TE applications. However, most of them possess TE figures of merit (ZT) that are below the applicable value of 2, in the mid-temperature region (from 250 to 600 °C). In a previous work, the removal of a small amount of Bi from BiCuSeO was found to improve the ZT of BiCuSeO. In this work, we pursue another track and study the TE performance of BiCuTeO after the addition of up to 6% excess Bi. Bi1+xCuTeO (x = 0.00–0.06) samples were prepared by solid-state reactions, followed by hot-pressing to form pellets. By adding a stoichiometric excess of Bi into BiCuTeO, 16% enhancement in power factor was achieved at 450 °C. This enhancement can be attributed to the increase in the Seebeck coefficient because of the appearance of secondary phases. Detailed characterizations and discussions of the effect of the nominal excess Bi in BiCuTeO are presented in this paper. The findings of this study can be applied in the investigation of novel high-performance TE materials.

A highly reproducible sample preparation method for pure GeTe in a rhombohedral structure without converting to the cubic structure up to ∼500 °C is reported to show control of the Ge-vacancy level and the corresponding herringbone-structured microdomains. The thermoelectric figure-of-merit (ZT) for GeTe powder could be raised from ∼0.8 to 1.37 at high temperature (HT) near ∼500 °C by tuning the Ge-vacancy level through the applied reversible in situ route, which made it highly controllable and reproducible. The enhanced ZT of GeTe was found to be strongly correlated with both its significantly increased Seebeck coefficient (∼161 μV K−1 at 500 °C) and reduced thermal conductivity (∼2.62 W m−1 K−1 at 500 °C) for a sample with nearly vacancy-free thicker herringbone-structured microdomains in the suppressed rhombohedral-to-cubic structure phase transformation. The microdomain and crystal structures were identified with HR-TEM (high-resolution transmission electron microscopy) and powder X-ray diffraction (XRD), while electron probe micro-analysis (EPMA) was used to confirm the stoichiometry changes of Ge : Te. Theoretical calculations for GeTe with various Ge-vacancy levels suggested that the Fermi level shifts toward the valence band as a function of increasing the Ge-vacancy level, which is consistent with the increased hole-type carrier concentration (n) and effective mass (m*) deduced from the Hall measurements. The uniquely prepared sample of a near-vacancy-free GeTe in a rhombohedral structure at high temperature favoured an enhanced Seebeck coefficient in view of the converging L- and Σ-bands of the heavy effective mass at the Fermi level, while the high density domain boundaries for the domain of low carrier density were shown to reduce the total thermal conductivity effectively.

BiCuTeO is a potential thermoelectric material owing to its low thermal conductivity and high carrier concentration. However, the thermoelectric performance of BiCuTeO is still below average and has much scope for improvement. In this study, we manipulated the nominal oxygen content in BiCuTeO and synthesized BiCuTeOx (x = 0.94–1.06) bulks by a solid-state reaction and pelletized them by a cold-press method. The power factor was enhanced by varying the nominal oxygen deficiency due to the increased Seebeck coefficient. The thermal conductivity was also reduced due to the decrease in lattice thermal conductivity owing to the small grain size generated by the optimal nominal oxygen content. Consequently, the ZT value was enhanced by ∼11% at 523 K for stoichiometric BiCuTeO0.94 compared to BiCuTeO. Thus, optimal oxygen manipulation in BiCuTeO can enhance the thermoelectric performance. This study can be applied to developing oxides with high thermoelectric performances.

Production of hydrogen from water electrolysis has stimulated the search of sustainable electrocatalysts as possible alternatives. Recently, cobalt phosphide (CoP) and molybdenum phosphide (MoP) received great attention owing to their superior catalytic activity and stability towards the hydrogen evolution reaction (HER) which rivals platinum catalysts. In this study, we synthesize and study a series of catalysts based on hybrids of CoP and MoP with different Co/Mo ratio. The HER activity shows a volcano shape and reaches a maximum for Co/Mo = 1. Tafel analysis indicates a change in the dominating step of Volmer-Hyrovský mechanism. Interestingly, X-ray diffraction patterns confirmed a major ternary interstitial hexagonal CoMoP(2) crystal phase is formed which enhances the electrochemical activity.