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Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals.

ABSTRACT: Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is important for heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density functional theory while retaining near DMC accuracy. Scrutinizing effects of energy dissipation and quantum tunneling, dynamics calculations suggest the approach to be of near chemical accuracy, reproducing molecular beam sticking experiments for the showcase H₂ + Al(110) system to ∼1.4 kcal/mol.

SUBMITTER: Powell AD

PROVIDER: S-EPMC10788952 | biostudies-literature | 2024 Jan

REPOSITORIES: biostudies-literature

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Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals.

Powell Andrew D AD Gerrits Nick N Tchakoua Theophile T Somers Mark F MF Busnengo Heriberto F HF Meyer Jörg J Kroes Geert-Jan GJ Doblhoff-Dier Katharina K

The journal of physical chemistry letters 20240103 1

Predictive capability, accuracy, and affordability are essential features of a theory that is capable of describing dissociative chemisorption on a metal surface. This type of reaction is important for heterogeneous catalysis. Here we present an approach in which we use diffusion Monte Carlo (DMC) to pin the minimum barrier height and construct a density functional that reproduces this value. This predictive approach allows the construction of a potential energy surface at the cost of density fu ...[more]

PMID: 38169287

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Project description:Abstract Biceps tendinopathy and superior labrum anterior posterior lesions are a common source of shoulder pain and disability and can be effectively treated with biceps tenodesis. There are a variety of open and arthroscopic tenodesis techniques, but no one technique has demonstrated superiority. Arthroscopic techniques often disregard the extra-articular portions of the biceps tendon as a potential source of pain. Open techniques address this concern; however, they can be associated with wound complications, increased blood loss, nerve injury, and disruptions to surgical workflow. Here, we describe an all arthroscopic tenodesis technique at the suprapectoral zone of the tendon. This method addresses extra-articular sources of pain, while limiting the potential pitfalls of open surgery. Technique Video Video 1 Narrated technique video. Standard posterior, anterior, lateral, and low anterior portals are used during the technique. Viewing from the posterior portal in a right shoulder the biceps anchor is debrided to a stable base. A BirdBeak device is inserted through the standard anterior portal and pierces the biceps tendon as laterally as possible, and an 18-gauge spinal needle is used to tease the suture from the BirdBeak device. After a standard subacromial decompression is performed the camera is inserted into the standard lateral portal, and an anterior subdeltoid bursectomy is performed to provide adequate visualization of the tenodesis site. An accessory low anterior portal is created about 1.5 cm proximal to the pectoralis major tendon insertion. The pectoralis major insertion site is used to aid in localization of the tendon just proximal to the subdeltoid portion of the tendon. An 11-blade is inserted through the low anterior portal and used to incise the transverse humeral ligament; the biceps tendon will often bulge from beneath the ligament at this step, confirming appropriate position. The bicep tendon is retracted with the probe, and a noncannulated 8-mm reamer is inserted into the low anterior portal and used to produce a unicortical tunnel. The tunnel’s edges are debrided using an arthroscopic shaver and the arthroscopic electrocautery device; the inferior portion of the tunnel must be smooth to prevent fraying of the tendon. The biceps tendon is then tensioned appropriately via tension pulled through the previously placed suture. A fork-tipped interference screw is then introduced through the low anterior portal to introduce the biceps tendon into the tenodesis site. The interference screw is then inserted and left 1 mm proud. The residual proximal bicep tendon is then amputated using an arthroscopic biter and removed through the lateral portal. The finished tenodesis site is probed and inspected, and a standard postoperative protocol is used.

Project description:PurposeHybrid image-guided surgery technologies such as combined radio- and fluorescence-guidance are increasingly gaining interest, but their added value still needs to be proven. In order to evaluate if and how fluorescence-guidance can help realize improvements beyond the current state-of-the-art in sentinel node (SN) biopsy procedures, use of the hybrid tracer indocyanine green (ICG)-99mTc-nancolloid was evaluated in a large cohort of patients.Patients and methodsA prospective trial was conducted (n = 501 procedures) in a heterogeneous cohort of 495 patients with different malignancies (skin malignancies, oral cavity cancer, penile cancer, prostate cancer and vulva cancer). After injection of ICG-99mTc-nanocolloid, SNs were preoperatively identified based on lymphoscintigraphy and SPECT/CT. Intraoperatively, SNs were pursued via gamma tracing, visual identification (blue dye) and/or near-infrared fluorescence imaging during either open surgical procedures (head and neck, penile, vulvar cancer and melanoma) or robot assisted laparoscopic surgery (prostate cancer). As the patients acted as their own control, use of hybrid guidance could be compared to conventional radioguidance and the use of blue dye (n = 300). This was based on reported surgical complications, overall survival, LN recurrence free survival, and false negative rates (FNR).ResultsA total of 1,327 SN-related hotspots were identified on 501 preoperative SPECT/CT scans. Intraoperatively, a total number of 1,643 SNs were identified based on the combination of gamma-tracing (>98%) and fluorescence-guidance (>95%). In patients wherein blue dye was used (n = 300) fluorescence-based SN detection was superior over visual blue dye-based detection (22-78%). No adverse effects related to the use of the hybrid tracer or the fluorescence-guidance procedure were found and outcome values were not negatively influenced.ConclusionWith ICG-99mTc-nanocolloid, the SN biopsy procedure has become more accurate and independent of the use of blue dye. With that, the procedure has evolved to be universal for different malignancies and anatomical locations.

Dataset Information

Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals.

Publications

Best-of-Both-Worlds Predictive Approach to Dissociative Chemisorption on Metals.

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