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"Wu, Tai"
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In situ X-ray spectroscopies beyond conventional X-ray absorption spectroscopy on deciphering dynamic configuration of electrocatalysts
by
Chen, Hao Ming
,
Hsu, Chia-Shuo
,
Chan, Ting-Shan
in
639/4077/909
,
639/638/161/886
,
Absorption spectroscopy
2023
Realizing viable electrocatalytic processes for energy conversion/storage strongly relies on an atomic-level understanding of dynamic configurations on catalyst-electrolyte interface. X-ray absorption spectroscopy (XAS) has become an indispensable tool to in situ investigate dynamic natures of electrocatalysts but still suffers from limited energy resolution, leading to significant electronic transitions poorly resolved. Herein, we highlight advanced X-ray spectroscopies beyond conventional XAS, with emphasis on their unprecedented capabilities of deciphering key configurations of electrocatalysts. The profound complementarities of X-ray spectroscopies from various aspects are established in a probing energy-dependent “in situ spectroscopy map” for comprehensively understanding the solid-liquid interface. This perspective establishes an indispensable in situ research model for future studies and offers exciting research prospects for scientists and spectroscopists.
X-ray absorption spectroscopy (XAS) has become an indispensable tool to investigate dynamic natures of electrocatalysts. In this perspective, advanced X-ray spectroscopies are highlighted in a complementary way, providing a promising research model for solid-liquid interface and (electro)catalysis studies.
Journal Article
Large-area, untethered, metamorphic, and omnidirectionally stretchable multiplexing self-powered triboelectric skins
2024
Large-area metamorphic stretchable sensor networks are desirable in haptic sensing and next-generation electronics. Triboelectric nanogenerator-based self-powered tactile sensors in single-electrode mode constitute one of the best solutions with ideal attributes. However, their large-area multiplexing utilizations are restricted by severe misrecognition between sensing nodes and high-density internal circuits. Here, we provide an electrical signal shielding strategy delivering a large-area multiplexing self-powered untethered triboelectric electronic skin (UTE-skin) with an ultralow misrecognition rate (0.20%). An omnidirectionally stretchable carbon black-Ecoflex composite-based shielding layer is developed to effectively attenuate electrostatic interference from wirings, guaranteeing low-level noise in sensing matrices. UTE-skin operates reliably under 100% uniaxial, 100% biaxial, and 400% isotropic strains, achieving high-quality pressure imaging and multi-touch real-time visualization. Smart gloves for tactile recognition, intelligent insoles for gait analysis, and deformable human-machine interfaces are demonstrated. This work signifies a substantial breakthrough in haptic sensing, offering solutions for the previously challenging issue of large-area multiplexing sensing arrays.
Stretchable sensor networks with multiplexing designs can result in misrecognition due to electrical signal interferences from the sensing nodes and internal circuits. Here, Shao et al. show an untethered triboelectric electronic skin with an elastic composite-based shield layer for lower misrecognition rate.
Journal Article
Self- regeneration of Au/CeO2 based catalysts with enhanced activity and ultra-stability for acetylene hydrochlorination
by
Zheng, Jianwei
,
Tsang, Shik Chi Edman
,
Ayvalı, Tuğçe
in
147/137
,
639/638/77/885
,
639/638/77/887
2019
Replacement of Hg with non-toxic Au based catalysts for industrial hydrochlorination of acetylene to vinyl chloride is urgently required. However Au catalysts suffer from progressive deactivation caused by auto-reduction of Au(I) and Au(III) active sites and irreversible aggregation of Au(0) inactive sites. Here we show from synchrotron X-ray absorption, STEM imaging and DFT modelling that the availability of ceria(110) surface renders Au(0)/Au(I) as active pairs. Thus, Au(0) is directly involved in the catalysis. Owing to the strong mediating properties of Ce(IV)/Ce(III) with one electron complementary redox coupling reactions, the ceria promotion to Au catalysts gives enhanced activity and stability. Total pre-reduction of Au species to inactive Au nanoparticles of Au/CeO
2
&AC when placed in a C
2
H
2
/HCl stream can also rapidly rejuvenate. This is dramatically achieved by re-dispersing the Au particles to Au(0) atoms and oxidising to Au(I) entities, whereas Au/AC does not recover from the deactivation.
Despite the extensive efforts to stabilize Au catalysts for industrial hydrochlorination of acetylene to vinyl chloride the deactivation is not overcome yet. Here, the authors demonstrate that the ceria promotion to Au catalysts affords enhanced activity and stability via formation of Au(0)/Au(I) as new active pairs.
Journal Article
Highly defective graphene quantum dots-doped 1T/2H-MoS2 as an efficient composite catalyst for the hydrogen evolution reaction
2023
We present a new composite catalyst system of highly defective graphene quantum dots (HDGQDs)-doped 1T/2H-MoS
2
for efficient hydrogen evolution reactions (HER). The high electrocatalytic activity, represented by an overpotential of 136.9 mV and a Tafel slope of 57.1 mV/decade, is due to improved conductivity, a larger number of active sites in 1T-MoS
2
compared to that in 2H-MoS
2
, and additional defects introduced by HDGQDs. High-resolution transmission electron microscopy (HRTEM), Raman spectroscopy, x-ray diffraction (XRD) and x-ray photoelectron spectroscopy (XPS) were used to characterize both the 1T/2H-MoS
2
and GQDs components while Fourier-transform infrared spectroscopy (FTIR) was employed to identify the functional groups on the edge and defect sites in the HDGQDs. The morphology of the composite catalyst was also examined by field emission scanning electron microscopy (FESEM). All experimental data demonstrated that each component contributes unique advantages that synergistically lead to the significantly improved electrocatalytic activity for HER in the composite catalyst system.
Journal Article
Hydrogen radical-boosted electrocatalytic CO2 reduction using Ni-partnered heteroatomic pairs
2024
The electrocatalytic reduction of CO
2
to CO is slowed by the energy cost of the hydrogenation step that yields adsorbed *COOH intermediate. Here, we report a hydrogen radical (H•)-transfer mechanism that aids this hydrogenation step, enabled by constructing Ni-partnered hetero-diatomic pairs, and thereby greatly enhancing CO
2
-to-CO conversion kinetics. The partner metal to the Ni (denoted as M) catalyzes the Volmer step of the water/proton reduction to generate adsorbed *H, turning to H•, which reduces CO
2
to carboxyl radicals (•COOH). The Ni partner then subsequently adsorbs the •COOH in an exothermic reaction, negating the usual high energy-penalty for the electrochemical hydrogenation of CO
2
. Tuning the H adsorption strength of the M site (with Cd, Pt, or Pd) allows for the optimization of H• formation, culminating in a markedly improved CO
2
reduction rate toward CO production, offering 97.1% faradaic efficiency (FE) in aqueous electrolyte and up to 100.0% FE in an ionic liquid solution.
Commercially viable catalytic CO
2
electroreduction to CO would enable many green technologies, yet it is impeded by the initial hydrogenation step of CO
2
. Here, the authors report Ni-Cd dual atom catalysts with complementary properties of favorable adsorption of CO
2
and H to overcome this barrier.
Journal Article
A cross-sectional study about the relationship between physical activity and sarcopenia in Taiwanese older adults
2021
To the best of our knowledge, none of Taiwanese studies on the relationship between physical activity (PA) and sarcopenia by the latest 2019 Asian Working Group for Sarcopenia (AWGS) cutoff points of sarcopenia has been published. We used the Taiwan version of international physical activity questionnaire-short version and the 2019 AWGS diagnostic criteria of sarcopenia to examine the relationship between PA and sarcopenia in older adults. Volunteers in this cross-sectional study were recruited from those attending senior health checkup program held at a regional hospital in Taipei City from May 2019 to Sep 2019. Muscle strength was assessed by grip strength, physical performance was assessed by usual gait speed on a 6-m course, and muscle mass was measured by bioelectrical impedance analysis. Multiple logistic regression was used to analyze the relationship between PA and sarcopenia. Odds ratios and corresponding 95% confidence intervals were calculated. 565 participants were recruited and data from 500 participants were used. The study participants had a mean age of 73.87 years old, with 47% men and 53% women. 138 (27.6%) participants were classified as having sarcopenia, among which 48 (45.3%) in low PA participants and 90 (22.8%) in moderate to high PA participants. Compared with those with low PA, moderate to high PA protected against the risk of sarcopenia with the odds ratio (OR) 0.46 (95% CI 0.27–0.79, p-value = 0.005). A significant protective effect of PA on sarcopenia was found among the older adults after adjusting for sex, institutionalization, age, BMI, albumin, hemoglobin, HDL-C levels, history of cardiovascular disease, education level and alcohol drinking.
Journal Article
Incidence and outcomes of acute kidney injury in extremely-low-birth-weight infants
by
Chan, Oi-Wa
,
Lee, Chien-Chung
,
Hsu, Kai-Hsiang
in
Acute kidney failure
,
Acute Kidney Injury - epidemiology
,
Acute Kidney Injury - pathology
2017
Acute kidney injury (AKI) is a common event in the neonatal intensive care unit (NICU), especially in extremely-low-birth-weight (ELBW) infants. This cohort study investigated the incidence of and risk factors for AKI in ELBW infants and their overall survival at the postmenstrual age (PMA) of 36 weeks.
All ELBW infants admitted to our NICU between January 2010 and December 2013 were enrolled. Those who died prior to 72 hours of life, had congenital renal abnormality, or had only one datum of the serum creatinine (SCr) level after the first 24 hours of life were excluded. The criteria used for the diagnosis of AKI was set according to the modified neonatal KDIGO AKI definition.
AKI occurred in 56% of 276 infants. Specifically, stage 1, stage 2, and stage 3 AKI occurred in 30%, 17%, and 9% of ELBW infants, respectively. High-frequency ventilation support (adjusted odds ratio [OR]: 3.4, 95% confidence interval [CI]: 1.78-6.67, p< 0.001), the presence of patent ductus arteriosus (adjusted OR: 4.3, 95% CI: 2.25-8.07, p < 0.001), lower gestational age (adjusted OR for gestational age: 0.7, 95% CI: 0.58-0.83, < 0.001), and inotropic agent use (adjusted OR: 2.6, 95% CI: 1.31-5.21, p = 0.006) were independently associated with AKI. Maternal pre-eclampsia was a protective factor (adjusted OR: 0.4, 95% CI: 0.14-0.97, p = 0.044). Infants with AKI had higher mortality before the PMA of 36 weeks with an adjusted hazard ratio (HR) of 5.34 (95% CI: 1.21-23.53, p = 0.027). Additionally, infants with stage 3 AKI had a highest HR of 10.60, 95% CI: 2.09-53.67, p = 0.004).
AKI was a very common event (56%) in ELBW infants and was associated with a lower GA, high-frequency ventilation support, the presence of PDA, and inotropic agent use. AKI reduced survival of ELBW infants before the PMA of 36 weeks.
Journal Article
Relationships among organizational culture, knowledge sharing, and innovation capability: a case of the automobile industry in Taiwan
2017
The advancement of automobiles (thereinafter auto) during these decades has not only made great contributions to the economic development, but also significantly changed people's life. Apparently, the auto industry has entered an innovation race. Among extant literature, organizational culture (OC) has positive impact on innovation capability (INC), whereas little research concerns about how OC influences organization's capabilities through knowledge management (KM) activities, especially for knowledge sharing (KS) taken in a firm. This study aims to explore the effect of OC and KS on INC in the knowledge-intensive auto industry. Questionnaires are given to 6 whole-car manufacturers, 49 parts suppliers, and 7 car dealers in Taiwan. 449 valid questionnaires are returned, and an empirical analysis through structural equation modeling (SEM) is performed. The result shows that KS is the mediating variable of OC and INC, and OC has a significant positive effect on KS.
Journal Article
Synthesis of core@shell catalysts guided by Tammann temperature
2024
Designing high-performance thermal catalysts with stable catalytic sites is an important challenge. Conventional wisdom holds that strong metal-support interactions can benefit the catalyst performance, but there is a knowledge gap in generalizing this effect across different metals. Here, we have successfully developed a generalizable strong metal-support interaction strategy guided by Tammann temperatures of materials, enabling functional oxide encapsulation of transition metal nanocatalysts. As an illustrative example, Co@BaAl
2
O
4
core@shell is synthesized and tracked in real-time through in-situ microscopy and spectroscopy, revealing an unconventional strong metal-support interaction encapsulation mechanism. Notably, Co@BaAl
2
O
4
exhibits exceptional activity relative to previously reported core@shell catalysts, displaying excellent long-term stability during high-temperature chemical reactions and overcoming the durability and reusability limitations of conventional supported catalysts. This pioneering design and widely applicable approach has been validated to guide the encapsulation of various transition metal nanoparticles for environmental tolerance functionalities, offering great potential to advance energy, catalysis, and environmental fields.
The authors report a synthetic strategy to create core@shell catalysts using strong metal-support interactions and low-Tammann-temperature compounds. The resulting materials are highly stable and may be useful in industrial applications.
Journal Article
General Strategy toward Hydrophilic Single Atom Catalysts for Efficient Selective Hydrogenation
2022
Well dispersible and stable single atom catalysts (SACs) with hydrophilic features are highly desirable for selective hydrogenation reactions in hydrophilic solvents towards important chemicals and pharmaceutical intermediates. A general strategy is reported for the fabrication of hydrophilic SACs by cation‐exchange approach. The cation‐exchange between metal ions (M = Ni, Fe, Co, Cu) and Na+ ions introduced in the skeleton of metal oxide (TiO2 or ZrO2) nanoshells plays the key role in forming M1/TiO2 and M1/ZrO2 SACs, which efficiently prevents the aggregation of the exchanged metal ions. The as‐obtained SACs are highly dispersible and stable in hydrophilic solvents including alcohol and water, which greatly facilitates the catalysis reaction in alcohol. The Ni1/TiO2 SACs have been successfully utilized as catalysts for the selective C=C hydrogenation of cinnamaldehyde to produce phenylpropanal with 98% conversion, over 90% selectivity, good recyclability, and a turnover frequency (TOF) of 102 h−1, overwhelming most reported catalysts including noble metal catalysts. A universal “cation‐exchange” strategy has been presented for the preparation of single‐atom catalysts (SACs) on various metal oxides with hydrophilic features. The Ni1/TiO2 SACs have demonstrated excellent catalytic performance for the selective hydrogenation of C=C in cinnamaldehyde to produce phenylpropanal in isopropanol, with high conversion and selectivity, good recyclability, and a turnover frequency (TOF) of up to 102 h−1.
Journal Article